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JP7606082B2 - Method for manufacturing wavelength conversion member and wavelength conversion member - Google Patents
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JP7606082B2 - Method for manufacturing wavelength conversion member and wavelength conversion member - Google Patents

Method for manufacturing wavelength conversion member and wavelength conversion member Download PDF

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JP7606082B2
JP7606082B2 JP2021008171A JP2021008171A JP7606082B2 JP 7606082 B2 JP7606082 B2 JP 7606082B2 JP 2021008171 A JP2021008171 A JP 2021008171A JP 2021008171 A JP2021008171 A JP 2021008171A JP 7606082 B2 JP7606082 B2 JP 7606082B2
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sintered body
light
wavelength conversion
conversion member
reflecting
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JP2022017160A (en
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利章 山下
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Nichia Corp
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Nichia Corp
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Priority to US17/371,342 priority Critical patent/US11920068B2/en
Priority to DE102021117776.6A priority patent/DE102021117776A1/en
Priority to CN202110784083.8A priority patent/CN113937611A/en
Publication of JP2022017160A publication Critical patent/JP2022017160A/en
Priority to US18/423,478 priority patent/US12173208B2/en
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Description

本開示は、波長変換部材の製造方法と波長変換部材に関する。 This disclosure relates to a method for manufacturing a wavelength conversion member and a wavelength conversion member.

近年、発光ダイオードやレーザダイオード等の光源を用いた白色照明が用いられるようになってきている。この白色照明の白色光は、例えば、発光ダイオードが発光する青色の光を波長変換部材により波長変換することにより得られる。特許文献1には、波長変換部材として、アルミナのセラミックマトリクスにYAG蛍光体粒子を分散させた焼結体が開示されている。 In recent years, white light illumination using light sources such as light-emitting diodes and laser diodes has come into use. The white light of this white light illumination is obtained, for example, by converting the wavelength of blue light emitted by a light-emitting diode using a wavelength conversion material. Patent Document 1 discloses a sintered body in which YAG phosphor particles are dispersed in an alumina ceramic matrix as a wavelength conversion material.

特開2016-204563号公報JP 2016-204563 A

このような、蛍光体粒子を含む焼結体は、例えば、光入射面から入射した光を入射光とは波長の異なる光に波長変換して光出射面から出射する光学部品に使用されるが、その際、光入射面及び光出射面以外の表面を反射部材によって覆うことにより光を効率良く波長変換できるよう構成される。なお、本明細書において、波長変換部材とは焼結体を含む部材を意味し、焼結体単体の場合もあれば、焼結体と反射部材等の他の部材を含む場合もある。
しかしながら、近年、波長変換部材が種々の用途に幅広く使用されるようになるに伴い、その光入射面及び光出射面以外の表面の光の閉じ込めの向上が求められるようになってきている。
そこで、本開示は光入射面及び光出射面以外の表面の光の閉じ込めが向上した焼結体を作製できる波長変換部材の製造方法と波長変換部材を提供することを目的とする。
Such a sintered body containing phosphor particles is used, for example, in an optical component that converts the light incident from a light incident surface into light having a different wavelength from the incident light and emits it from a light exit surface, and in this case, the surface other than the light incident surface and the light exit surface is covered with a reflecting member so that the light can be efficiently wavelength-converted. Note that in this specification, the wavelength conversion member means a member containing a sintered body, and may be a single sintered body or may include a sintered body and other members such as a reflecting member.
However, in recent years, as wavelength conversion members have come to be widely used for various applications, there has been a demand for improving the light confinement on surfaces other than the light entrance surface and the light exit surface.
Therefore, an object of the present disclosure is to provide a manufacturing method for a wavelength conversion member that can produce a sintered body with improved light confinement on surfaces other than the light entrance surface and light exit surface, and a wavelength conversion member.

以上の課題を解決するために、本開示に係る波長変換部材の製造方法は、
光入射面と、光出射面と、前記光入射面及び光出射面とは異なる面である光反射面とを備える焼結体を含む波長変換部材の製造方法であって、
無機物粒子と蛍光体粒子とを含む焼結体を準備する焼結体準備工程と、
前記焼結体を酸処理し、前記焼結体の光反射面に複数の凹部を形成する凹部形成工程と、
を含む。
In order to solve the above problems, the method for producing a wavelength conversion member according to the present disclosure includes:
A method for producing a wavelength conversion member including a sintered body having a light incident surface, a light exit surface, and a light reflecting surface that is different from the light incident surface and the light exit surface, comprising:
a sintered body preparation step of preparing a sintered body containing inorganic particles and phosphor particles;
a recess forming step of treating the sintered body with acid to form a plurality of recesses on a light reflecting surface of the sintered body;
Includes.

以上のように構成された本開示に係る波長変換部材の製造方法は、無機物粒子と蛍光体粒子とを含む焼結体を準備して、該焼結体を酸処理して焼結体の光反射面に複数の凹部を形成する工程を含むので、光入射面及び光出射面以外の表面の光の閉じ込めが向上した焼結体を作製でき、当該焼結体を含む波長変換部材を作製することが可能になる。 The method for producing a wavelength conversion member according to the present disclosure configured as described above includes the steps of preparing a sintered body containing inorganic particles and phosphor particles, and treating the sintered body with acid to form multiple recesses on the light reflecting surface of the sintered body, so that a sintered body with improved light confinement on surfaces other than the light entrance surface and light exit surface can be produced, and a wavelength conversion member including the sintered body can be produced.

本発明に係る実施形態1の製造方法のフローである。1 is a flow chart of a manufacturing method according to a first embodiment of the present invention. 実施形態1の製造方法における焼結体準備工程のフローである。4 is a flow chart of a sintered body preparation process in the manufacturing method of embodiment 1. 実施形態1の製造方法において、準備した焼結体の断面図である。2 is a cross-sectional view of a sintered body prepared in the manufacturing method of embodiment 1. FIG. 実施形態1の製造方法において、凹部を形成した焼結体の断面図である。4 is a cross-sectional view of a sintered body having a recess formed therein in the manufacturing method of embodiment 1. FIG 実施形態1の製造方法において、凹部を形成した焼結体を反射部材で取り囲んだときの断面図である。4 is a cross-sectional view showing a state in which a sintered body having a recess formed therein is surrounded by a reflecting member in the manufacturing method of the first embodiment. FIG. 実施形態1の製造方法において、凹部を形成した焼結体を含む反射部材を加工した波長変換部材集合体の断面図である。4 is a cross-sectional view of a wavelength conversion member assembly obtained by processing a reflecting member including a sintered body having recesses formed therein in the manufacturing method of embodiment 1. FIG. 図3Dの波長変換部材集合体の平面図である。FIG. 3E is a plan view of the wavelength conversion member assembly of FIG. 3D. 実施形態1の製造方法において、波長変換部材集合体を個片化した後の波長変換部材の平面図である。10 is a plan view of a wavelength conversion member after the wavelength conversion member assembly is divided into individual pieces in the manufacturing method of embodiment 1. FIG. 実施形態1の製造方法により作製された波長変換部材の応用例の模式図である。4A to 4C are schematic diagrams of application examples of a wavelength conversion member produced by the manufacturing method of embodiment 1. 焼結体中の蛍光体粒子の分布を評価する方法を説明するための簡略化した模式的な断面図である。FIG. 11 is a simplified schematic cross-sectional view for explaining a method for evaluating the distribution of phosphor particles in a sintered body. 実施形態2の製造方法において、準備した焼結体の断面図である。FIG. 11 is a cross-sectional view of a sintered body prepared in the manufacturing method of embodiment 2. 実施形態2の製造方法において、凹部を形成した焼結体の断面図である。FIG. 11 is a cross-sectional view of a sintered body having a recess formed therein in the manufacturing method of embodiment 2. 実施形態2の製造方法において、形成した凹部の一部を除去した後の焼結体の断面図である。FIG. 11 is a cross-sectional view of a sintered body after a portion of a formed recess is removed in a manufacturing method of embodiment 2. 実施形態2の製造方法において、焼結体の凸部を個片化した後の焼結体の断面図である。11 is a cross-sectional view of a sintered body after the protrusions of the sintered body are singulated in the manufacturing method of embodiment 2. FIG. 実施形態2の製造方法において、準備した反射部材の断面図である。13 is a cross-sectional view of a prepared reflective member in a manufacturing method according to a second embodiment. FIG. 実施形態2の製造方法において、準備した反射部材の貫通孔に個片化した後の焼結体を挿入した後の断面図である。13 is a cross-sectional view of the prepared reflective member after an individualized sintered body is inserted into a through hole in the reflective member in the manufacturing method of embodiment 2. FIG. 実施形態2の製造方法において、貫通孔に挿入した焼結体の上にガラスを設けた後の断面図である。13 is a cross-sectional view of the manufacturing method of the second embodiment after glass is provided on the sintered body inserted into the through hole. FIG. 実施形態2の製造方法において、ガラスの表面を研磨した後の断面図である。FIG. 11 is a cross-sectional view of the glass after the surface of the glass is polished in the manufacturing method of the embodiment 2. 実施形態2の製造方法により作製された波長変換部材の応用例の模式図である。11A to 11C are schematic diagrams of application examples of a wavelength conversion member produced by the production method of embodiment 2. 本発明に係る実施形態3の製造方法のフローである。13 is a flow chart of a manufacturing method according to a third embodiment of the present invention. 実施形態3の製造方法において、上面にマスクが形成され、下面に保護膜が形成された蛍光体セラミック板の断面図である。11 is a cross-sectional view of a phosphor ceramic plate having a mask formed on its upper surface and a protective film formed on its lower surface in a manufacturing method according to a third embodiment. FIG. 図6Aの蛍光体セラミック板の平面図である。FIG. 6B is a plan view of the phosphor ceramic plate of FIG. 6A. 実施形態3の製造方法において、凹部を形成した蛍光体セラミック板の断面図である。13 is a cross-sectional view of a phosphor ceramic plate having recesses formed therein in a manufacturing method according to a third embodiment. FIG. 実施形態3の製造方法において、蛍光体セラミック板の下面全体に反射膜を形成したときの断面図である。13 is a cross-sectional view showing a state in which a reflective film is formed on the entire lower surface of a phosphor ceramic plate in the manufacturing method of embodiment 3. FIG. 実施形態3の製造方法において、蛍光体セラミック板を下面側から支持する支持体を設けたときの断面図である。13 is a cross-sectional view showing a state where a support body is provided to support the phosphor ceramic plate from the lower surface side in the manufacturing method of the third embodiment. FIG. 実施形態3の製造方法により作製された波長変換部材の応用例の模式図である。13A to 13C are schematic diagrams of application examples of a wavelength conversion member produced by the manufacturing method of embodiment 3. 実験例と同様にして作製した焼結体の光反射面に反射部材を形成したときの断面写真である。13 is a cross-sectional photograph of a sintered body produced in the same manner as in the experimental example, when a reflecting member is formed on the light reflecting surface of the sintered body. 図7Aから反射部材を除いた焼結体の断面写真である。7B is a cross-sectional photograph of the sintered body from which the reflective member has been removed, FIG. 7A. 比較例と同様にして作製した焼結体の光反射面に反射部材を形成したときの断面写真である。13 is a cross-sectional photograph of a sintered body produced in the same manner as in the comparative example, when a reflective member is formed on the light-reflecting surface of the sintered body.

本開示に係る波長変換部材の製造方法は、無機物粒子と蛍光体粒子とを含む焼結体を酸処理することによりその酸処理された表面の光の閉じ込めが向上することを見いだし完成させたものであり、少なくとも無機物粒子と蛍光体粒子とを含む焼結体を準備する焼結体準備工程と凹部形成工程とを含む。
ここで、凹部形成工程は、準備した焼結体の表面を酸処理して、焼結体の光反射面に複数の凹部を形成する工程である。より具体的には、焼結体の表面を酸処理することにより、焼結体の光反射面に露出した蛍光体粒子を離脱させ、残った無機物粒子により形成された焼結体の光反射面に、複数の凹部を形成するものである。以上のように焼結体の光反射面に複数の凹部を形成することにより、光反射面における光の閉じ込めを向上させることができる。これは、光反射面における無機物粒子と凹部の空隙との間の屈折率差によるものと考えられる。また、光反射面に露出する蛍光体粒子が減少することによるものとも考えられる。
The method for manufacturing a wavelength conversion member according to the present disclosure was developed by discovering that acid-treating a sintered body containing inorganic particles and phosphor particles improves light confinement on the acid-treated surface, and includes a sintered body preparation step of preparing a sintered body containing at least inorganic particles and phosphor particles, and a recess formation step.
Here, the recess forming step is a step of acid-treating the surface of the prepared sintered body to form multiple recesses on the light-reflecting surface of the sintered body. More specifically, by acid-treating the surface of the sintered body, the phosphor particles exposed on the light-reflecting surface of the sintered body are removed, and multiple recesses are formed on the light-reflecting surface of the sintered body formed by the remaining inorganic particles. By forming multiple recesses on the light-reflecting surface of the sintered body as described above, it is possible to improve the confinement of light on the light-reflecting surface. This is thought to be due to the refractive index difference between the inorganic particles on the light-reflecting surface and the voids of the recesses. It is also thought to be due to a decrease in the phosphor particles exposed on the light-reflecting surface.

また、本開示に係る波長変換部材の製造方法は、焼結体において、光入射面及び光出射面として利用する面の光の閉じ込めを抑えるために、必要に応じて、以下の工程のいずれかを含んでいてもよい。
(a)凹部形成工程後に、酸処理により凹部が形成された表面のうち、光入射面及び光出射面として利用する面における凹部を除去する凹部除去工程。
(b)光入射面及び光出射面として利用する面が酸処理にさらされないように、凹部形成工程の前に、光入射面及び光出射面として利用する面にマスクを形成する工程。
Furthermore, the method for producing a wavelength conversion member according to the present disclosure may include any one of the following steps as necessary to suppress light confinement on the surfaces used as the light incident surface and the light exit surface of the sintered body.
(a) a recess removing step of removing the recesses from the surfaces to be used as the light incident surface and the light emitting surface, among the surfaces on which the recesses have been formed by the acid treatment after the recess forming step;
(b) A step of forming a mask on the surfaces to be used as the light incident surface and the light emitting surface, prior to the recess forming step, so as to prevent the surfaces from being exposed to the acid treatment.

本開示に係る波長変換部材の製造方法によれば、焼結体の表面のうち光入射面と光出射面とを除く表面を光の閉じ込めが向上した光反射面とすることが可能になる。以上のように作製された焼結体は、光入射面と光出射面とを除く表面が光の閉じ込めが向上した光反射面となっていることから、光入射面と光出射面とを除いた表面から漏れる光を少なくでき、光入射面から入射した光を効率良く波長変換して光出射面から出射させることができる。
なお、作製する焼結体の光入射面と光出射面とは異なる面であってもよいし、同一の面であってもよい。
According to the manufacturing method of the wavelength conversion member of the present disclosure, the surface of the sintered body, excluding the light incident surface and the light exit surface, can be made into a light reflecting surface with improved light confinement. Since the surface of the sintered body, excluding the light incident surface and the light exit surface, of the sintered body produced as described above is a light reflecting surface with improved light confinement, it is possible to reduce light leaking from the surface excluding the light incident surface and the light exit surface, and the light incident from the light incident surface can be efficiently wavelength converted and emitted from the light exit surface.
The light incident surface and the light emitting surface of the sintered body to be produced may be different surfaces or may be the same surface.

また、実施形態の波長変換部材の製造方法において、焼結体の光入射面と光出射面とを露出させ、かつ複数の凹部が形成された光反射面を接して覆う反射部材を設ける反射部材配置工程をさらに含むことにより、焼結体と反射部材とを含む波長変換部材を製造することができる。この焼結体と反射部材とを含む波長変換部材は、焼結体の光反射面における光の閉じ込めだけでなく、焼結体と反射部材との界面における光反射率を高くできることから、焼結体の光出射面の周りの光の滲みを抑制できる。これにより、焼結体の光出射面と、光出射面の外側とで輝度差を大きくでき、言い換えれば、焼結体の光出射面と該光出射面を取り囲む反射部材との境界を明瞭にでき、見切りに優れた波長変換部材を作製することができる。 In addition, in the manufacturing method of the wavelength conversion member of the embodiment, by further including a reflecting member arrangement step of exposing the light entrance surface and the light exit surface of the sintered body and providing a reflecting member that contacts and covers the light reflection surface on which the multiple recesses are formed, a wavelength conversion member including a sintered body and a reflecting member can be manufactured. This wavelength conversion member including a sintered body and a reflecting member can not only confine light in the light reflection surface of the sintered body, but also increase the light reflectance at the interface between the sintered body and the reflecting member, thereby suppressing light bleeding around the light exit surface of the sintered body. This makes it possible to increase the luminance difference between the light exit surface of the sintered body and the outside of the light exit surface, in other words, to clearly define the boundary between the light exit surface of the sintered body and the reflecting member surrounding the light exit surface, and thus to manufacture a wavelength conversion member with excellent visibility.

以下、実施形態の波長変換部材の製造方法について、図面を参照しながらより具体的な例を用いて詳細に説明する。
なお、以下に示す実施形態1~3の波長変換部材の製造方法は、反射部材配置工程を含むものであるが、反射部材配置工程は、必要に応じて設けられる工程であって任意である。すなわち、上述したように、実施形態の波長変換部材の製造方法により作製された、光反射面に複数の凹部が形成された焼結体は、光反射面での光の閉じ込めを向上できることから、光反射面を接して覆う反射部材を含むことなく光の閉じ込めを向上させることが可能であり、光反射面を覆う反射部材を含むことなく、波長変換部材として使用することができる。
また、以下の実施形態1~3は、上述した実施形態の技術思想を具体化したものであるが、本発明を限定するものではない。また、以下の説明において、同一の名称、符号については同一もしくは同質の部材を示しており、重複した説明は適宜省略することがある。なお、各図面が示す部材の大きさや位置関係等は、説明を明確にするために誇張していることがある。
Hereinafter, the method for producing a wavelength conversion member according to the embodiment will be described in detail using more specific examples with reference to the drawings.
The manufacturing method of the wavelength conversion member of the first to third embodiments described below includes a reflective member arrangement step, but the reflective member arrangement step is an optional step that is provided as necessary. That is, as described above, the sintered body having a plurality of recesses formed on the light reflecting surface produced by the manufacturing method of the wavelength conversion member of the embodiment can improve the light confinement on the light reflecting surface, and therefore can improve the light confinement without including a reflective member that contacts and covers the light reflecting surface, and can be used as a wavelength conversion member without including a reflective member that covers the light reflecting surface.
The following embodiments 1 to 3 embody the technical ideas of the above-mentioned embodiments, but do not limit the present invention. In the following description, the same names and symbols indicate the same or similar components, and duplicate descriptions may be omitted as appropriate. The sizes and positional relationships of the components shown in each drawing may be exaggerated to clarify the description.

実施形態1
実施形態1の波長変換部材1の製造方法は、図1に示すように、焼結体準備工程S1と、凹部形成工程S2と、反射部材配置工程S3とを含む。
EMBODIMENT 1
As shown in FIG. 1, the method for manufacturing wavelength conversion member 1 of embodiment 1 includes a sintered body preparing step S1, a recess forming step S2, and a reflecting member arranging step S3.

1.焼結体準備工程S1
焼結体準備工程S1は、図2に示すように、秤量工程S11と、混合工程S12と、成形工程S13と、焼結工程S14と、加工工程S15と、を含む。
以下、各工程について具体的に説明する。
1. Sintered body preparation step S1
As shown in FIG. 2, the sintered body preparation step S1 includes a weighing step S11, a mixing step S12, a molding step S13, a sintering step S14, and a processing step S15.
Each step will now be described in detail.

(1-1)秤量工程S11
ここでは、無機物粒子と蛍光体粒子とをそれぞれ準備し、準備した無機物粒子と蛍光体粒子とをそれぞれ所定量秤量する。なお、蛍光体粒子の準備には、蛍光体粒子そのものを準備することのほか、蛍光体粒子の原料となる材料を準備することも含む。例えば、YAG蛍光体粒子を準備する場合、酸化アルミニウム、酸化イットリウム及び酸化セリウムの粒子をそれぞれ準備してもよい。
(1-1) Weighing step S11
Here, inorganic particles and phosphor particles are prepared, and the inorganic particles and phosphor particles are weighed in a predetermined amount. The preparation of phosphor particles includes not only the preparation of phosphor particles themselves, but also the preparation of materials that are the raw materials of phosphor particles. For example, when preparing YAG phosphor particles, aluminum oxide, yttrium oxide, and cerium oxide particles may be prepared.

蛍光体粒子は、入射光により励起されて入射光より波長の長い光を発光するものであり、無機物粒子は焼結後に蛍光体粒子を支持するものである。 The phosphor particles are excited by incident light and emit light with a longer wavelength than the incident light, and the inorganic particles support the phosphor particles after sintering.

蛍光体粒子としては、例えば、セリウムで賦活されたYAG(Yttrium Aluminum Garnet)系蛍光体、ユウロピウム及び/又はクロムで賦活された窒素含有アルミノ珪酸カルシウム(CaO-Al-SiO)蛍光体、ユウロピウムで賦活されたシリケート((Sr,Ba)SiO)蛍光体、αサイアロン蛍光体、βサイアロン蛍光体等から選択された1又は2種以上からなる蛍光体粒子を準備する。蛍光体粒子としては、比較的耐熱性が高く、励起光による劣化の少ない材料を用いることが好ましく、好適な材料として、例えば、YAG系蛍光体が挙げられる。ここで、YAG系蛍光体には、例えばYの少なくとも一部をTbに置換したものや、Yの少なくとも一部をLuに置換したものも含まれる。また、YAG系蛍光体は、組成中にGdやGa等が含まれるものであってもよい。 The phosphor particles are prepared by using one or more phosphor particles selected from, for example, a cerium-activated YAG (Yttrium Aluminum Garnet) phosphor, a nitrogen-containing calcium aluminosilicate (CaO-Al 2 O 3 -SiO 2 ) phosphor activated with europium and/or chromium, a silicate ((Sr,Ba) 2 SiO 4 ) phosphor activated with europium, an α-sialon phosphor, a β-sialon phosphor, and the like. As the phosphor particles, it is preferable to use a material that is relatively heat-resistant and less likely to deteriorate due to excitation light, and a suitable material is, for example, a YAG phosphor. Here, the YAG phosphor includes, for example, one in which at least a part of Y is replaced with Tb, or one in which at least a part of Y is replaced with Lu. The YAG phosphor may also include Gd, Ga, or the like in its composition.

準備する蛍光体粒子の粒径は、例えば、0.1μm以上、30μm以下の範囲内であることが好ましく、1μm以上、5μm以下の範囲内とすることがさらに好ましい。この範囲とすることにより焼結体11の酸処理後の表面の光の閉じ込めをより向上させることができる。このとき、無機物粒子として、蛍光体粒子の焼結温度よりも低い焼結温度の無機物粒子を用いる。これにより、蛍光体粒子の熱による劣化を低減しながら無機物粒子を焼結することができる。 The particle size of the phosphor particles to be prepared is preferably, for example, in the range of 0.1 μm or more and 30 μm or less, and more preferably in the range of 1 μm or more and 5 μm or less. By setting the particle size in this range, it is possible to further improve the light confinement on the surface of the sintered body 11 after the acid treatment. In this case, inorganic particles with a sintering temperature lower than the sintering temperature of the phosphor particles are used as the inorganic particles. This allows the inorganic particles to be sintered while reducing the thermal deterioration of the phosphor particles.

また、無機物粒子として、例えば、酸化アルミニウムもしくは酸化イットリウム等の酸化物または窒化物等から選択された1又は2種以上からなる無機物粒子を準備する。無機物粒子として、蛍光体粒子の熱膨張係数に近い熱膨張係数の材料や、光吸収の少ない材料を用いることが好ましく、好適な材料として、例えば、酸化アルミニウムが挙げられる。
準備する無機物粒子の粒径は、蛍光体粒子の粒径より小さいことが好ましく、例えば、0.01μm以上、1μm以下の範囲内、より好ましくは、0.3μm以上、0.6μm以下の範囲内のものを用いる。無機物粒子の材料の選択に加え、蛍光体粒子の粒径より小さい粒子を選択することにより、無機物粒子の焼結温度を蛍光体粒子よりも低い焼結温度とすることができる。これにより、蛍光体粒子の熱による劣化及び異常な粒成長を抑制しながら無機物粒子を焼結させることができる。また、無機物粒子の粒径が小さすぎる場合、無機物粒子の凝集により、取り扱いが難しくなることや、混合ムラによる焼結ムラが起きることがあるので、この観点からは、粒径が0.1μm以上あることが好ましい。
なお、ここでいう粒径とは、平均粒径をいい、レーザ回折法により測定された粒径をいう。
In addition, inorganic particles made of one or more kinds selected from oxides such as aluminum oxide or yttrium oxide, nitrides, etc. are prepared as inorganic particles. It is preferable to use a material with a thermal expansion coefficient close to that of the phosphor particles or a material with low light absorption as the inorganic particles, and a suitable material is, for example, aluminum oxide.
The particle size of the inorganic particles to be prepared is preferably smaller than that of the phosphor particles, for example, in the range of 0.01 μm or more and 1 μm or less, more preferably 0.3 μm or more and 0.6 μm or less. In addition to the selection of the material of the inorganic particles, by selecting particles smaller than the particle size of the phosphor particles, the sintering temperature of the inorganic particles can be set to a lower sintering temperature than that of the phosphor particles. This allows the inorganic particles to be sintered while suppressing the deterioration of the phosphor particles due to heat and abnormal grain growth. In addition, if the particle size of the inorganic particles is too small, the inorganic particles may become difficult to handle due to aggregation, or uneven sintering may occur due to uneven mixing, so from this viewpoint, the particle size is preferably 0.1 μm or more.
The particle size referred to here means an average particle size, and is a particle size measured by a laser diffraction method.

次に、準備した無機物粒子及び蛍光体粒子を秤量する。
無機物粒子及び蛍光体粒子の合計重量に対して、無機物粒子及び蛍光体粒子がそれぞれ所定の重量比になるように秤量する。ここで、無機物粒子及び蛍光体粒子の合計重量に対する無機物粒子の重量比は、例えば、20%以上、95%以下の範囲、好ましくは60%以上、90%以下の範囲、より好ましくは70%以上、80%以下の範囲内で所望の波長変換特性が得られるように適宜設定される。
また、蛍光体粒子の粒径及び無機物粒子の粒径を上記範囲において適宜選択し、蛍光体粒子の量及び無機物粒子の量を上記範囲において適宜選択することにより、比較的粒径の小さい無機物粒子の中に蛍光体粒子を点在させることができ、後述の工程により無機物粒子が焼結してなる無機物マトリクスにより蛍光体粒子が支持された焼結体11を作製することができる。
Next, the prepared inorganic particles and phosphor particles are weighed.
The inorganic particles and the phosphor particles are weighed out so as to have a predetermined weight ratio with respect to the total weight of the inorganic particles and the phosphor particles. Here, the weight ratio of the inorganic particles to the total weight of the inorganic particles and the phosphor particles is appropriately set so as to obtain a desired wavelength conversion characteristic within a range of, for example, 20% or more and 95% or less, preferably 60% or more and 90% or less, more preferably 70% or more and 80% or less.
Furthermore, by appropriately selecting the particle size of the phosphor particles and the particle size of the inorganic particles within the above ranges, and by appropriately selecting the amount of the phosphor particles and the amount of the inorganic particles within the above ranges, the phosphor particles can be scattered among inorganic particles of relatively small particle size, and a sintered body 11 can be produced in which the phosphor particles are supported by an inorganic matrix formed by sintering the inorganic particles in the process described below.

(1-2)混合工程S12
次に、秤量した無機物粒子及び蛍光体粒子を、例えば、アルミナボールとともに混合容器に入れて回転させることにより混合する(ボールミル混合)。ボールミル混合はエタノール等の溶剤を含む湿式混合を用いてもよいし、溶剤を含まない乾式混合を用いてもよい。
(1-2) Mixing step S12
Next, the weighed inorganic particles and phosphor particles are mixed by, for example, placing them in a mixing vessel together with alumina balls and rotating them (ball mill mixing). The ball mill mixing may be performed using a wet mixing method that includes a solvent such as ethanol. Alternatively, a dry blend containing no solvent may be used.

(1-3)成形工程S13
ここでは、無機物粒子と蛍光体粒子とが混合された混合粉体を所定の形状に成形する。
成形工程S13は、例えば、一次成形工程S131と二次成形工程S132とを含む。
一次成形工程S131では、プレス成型等により上下から加圧して一次成形する。二次成形工程S132では、一次成形品をCIP(冷間静水圧加圧)成形等により等方的に加圧することにより加圧成形後の密度が均一になるように所定の形状に成形する。
(1-3) Molding process S13
Here, a powder mixture of inorganic particles and phosphor particles is molded into a predetermined shape.
The molding step S13 includes, for example, a primary molding step S131 and a secondary molding step S132.
In the primary molding step S131, pressure is applied from above and below by press molding or the like to perform primary molding. In the secondary molding step S132, the primary molded product is isotropically pressed by CIP (cold isostatic pressing) molding or the like to perform secondary molding. The material is molded into a desired shape so that the density after compression molding is uniform.

(1-4)焼結工程S14
焼結工程では、例えば、無機物粒子が酸化アルミニウムであれば、1300℃以上、1600℃以下程度の所定の焼結温度で一定時間保持することにより、無機物粒子を焼結させて蛍光体粒子を支持するマトリクス状の支持部を形成する。焼結工程S14は、例えば、所定の温度で大気圧中で焼結させる一次焼結工程S141と、一次焼結工程S141より高密度に焼結させることができる二次焼結工程S142とを含む。一次焼結工程S141では、放電プラズマ焼結(Spark Plasma Sinterning、SPS)法を用いることができる。二次焼結工程S142では、ホットプレス(HP)法、熱間静水圧加圧(HIP)法を用いることができる。焼結温度及び時間は、蛍光体粒子の熱による劣化及び異常な粒成長を抑制しつつ無機物粒子を焼結させるよう適宜設定する。
(1-4) Sintering step S14
In the sintering step, for example, if the inorganic particles are aluminum oxide, the inorganic particles are sintered by holding the inorganic particles at a predetermined sintering temperature of about 1300° C. or more and 1600° C. or less for a certain period of time to form a matrix-shaped support portion that supports the phosphor particles. The sintering step S14 includes, for example, a primary sintering step S141 in which sintering is performed at a predetermined temperature under atmospheric pressure, and a secondary sintering step S142 in which sintering can be performed at a higher density than the primary sintering step S141. In the primary sintering step S141, a spark plasma sintering (SPS) method can be used. In the secondary sintering step S142, a hot pressing (HP) method or a hot isostatic pressing (HIP) method can be used. The sintering temperature and time are appropriately set so as to sinter the inorganic particles while suppressing thermal deterioration and abnormal grain growth of the phosphor particles.

ここでの焼結温度及び時間は、無機物粒子の焼結後の結晶粒径及び蛍光体粒子の焼結後の粒径が所望の寸法になるように焼結前の無機物粒子の粒径及び焼結前の蛍光体粒子の粒径を考慮して適宜設定する。蛍光体粒子としてYAG系蛍光体、無機物粒子として酸化アルミニウムを選択して、ホットプレス(HP)法を用いる場合は、例えば、1350℃以上、1600℃以下の範囲内の温度で、その温度での保持時間は30分以上、600分以下の範囲内の時間行う。
なお、焼結体11の蛍光体粒子の結晶粒径の測定方法は、例えば、焼結体11の一断面において、蛍光体粒子が10個写るスケールのSEM画像で、円形に近い形状の蛍光体粒子のうち、最短の幅をもつものと最長の幅をもつものの平均を求めることにより測定することができる。以下の説明及び参照する図において、焼結体11中の蛍光体粒子には、17の符号を付して示す。
The sintering temperature and time are appropriately set in consideration of the particle size of the inorganic particles before sintering and the particle size of the phosphor particles before sintering so that the crystal particle size of the inorganic particles after sintering and the particle size of the phosphor particles after sintering are the desired size. When a YAG phosphor is selected as the phosphor particles and aluminum oxide is selected as the inorganic particles, and a hot press (HP) method is used, the sintering is performed at a temperature in the range of 1350° C. to 1600° C., for example, for a holding time at that temperature in the range of 30 minutes to 600 minutes.
The crystal grain size of the phosphor particles in the sintered body 11 can be measured, for example, by averaging the widths of the shortest and longest phosphor particles that are nearly circular in a SEM image of a scale that shows 10 phosphor particles in one cross section of the sintered body 11. In the following explanation and in the figures to be referred to, the phosphor particles in the sintered body 11 are indicated by the reference number 17.

(1-5)加工工程S15
得られた焼結体11を必要に応じて所定の形状に加工する。ここでは、例えば図3Aに示すように所定の寸法の四角柱形状に加工する。なお、加工後の焼結体11の表面は、図3Aに示すように実質的に平坦である。ここで、本明細書において実質的に平坦とは、焼結後の特に研削または研磨されていない通常の焼結体の表面状態のことをいう。
(1-5) Processing process S15
The obtained sintered body 11 is processed into a predetermined shape as required. For example, as shown in FIG. 3A, the sintered body 11 is processed into a square prism shape of a predetermined dimension. The surface is substantially flat as shown in Fig. 3A. In this specification, "substantially flat" refers to the surface state of a normal sintered body after sintering, which has not been ground or polished. This means.

2.凹部形成工程S2
凹部形成工程S2では、焼結体準備工程S1で準備した焼結体11を酸処理し、図3Bに示すように、焼結体11の表面に複数の凹部7を形成する。
ここでは、蛍光体粒子17または無機物粒子の少なくとも一方を溶解する溶液を用いる。好ましくは、無機物粒子の溶解率よりも、蛍光体粒子17の溶解率のほうが大きい溶液を用いる。このような溶液として、例えば、燐酸、硫酸、フッ酸、硝酸が挙げられる。
酸処理は、例えば、燐酸と硫酸の混合液を加熱して、その液中で所定の時間行い、その後水洗する。燐酸と硫酸の割合は、例えば、1:1~1:5、混合液の加熱温度は、例えば、100℃以上、320℃以下、処理時間は、例えば、1分以上、60分以下の範囲で、目標とする凹部7の形状および大きさ等を考慮して適宜設定される。以上の酸処理により、焼結体11の表面の無機物粒子と蛍光体粒子17の粒子間が優先的に溶解されて、再び粒状化される。換言すると、無機物粒子と蛍光体粒子17の粒子間が優先的に溶解されて、粒子の状態に戻る。そして、蛍光体粒子17が離脱して焼結体11の表面に凹部7が形成される。
例えば、YAGからなる蛍光体粒子17と酸化アルミニウムからなる無機物粒子とを含む焼結体11を、燐酸と硫酸が36:74で混合された混合液により酸処理する場合には、YAGは200℃の温度で溶解され、一方酸化アルミニウムは約260℃から溶解が始まるので、例えば、混合液の温度を280℃以上、305℃以下の範囲に設定する。このようにすると、酸化アルミニウムよりYAGの溶解率が大きいので、無機物粒子と蛍光体粒子17の粒子間において蛍光体粒子17の表面が優先的に溶解されて無機物粒子と蛍光体粒子17の間が分離されて蛍光体粒子17が離脱し、焼結体11の表面に凹部7が形成される。
2. Recess formation step S2
In the recess forming step S2, the sintered body 11 prepared in the sintered body preparing step S1 is treated with acid to form a plurality of recesses 7 on the surface of the sintered body 11 as shown in FIG. 3B.
Here, a solution that dissolves at least one of the phosphor particles 17 and the inorganic particles is used. Preferably, a solution in which the dissolution rate of the phosphor particles 17 is greater than the dissolution rate of the inorganic particles is used. For example, phosphoric acid, sulfuric acid, hydrofluoric acid, and nitric acid can be mentioned.
The acid treatment is carried out, for example, by heating a mixture of phosphoric acid and sulfuric acid, and then immersing the material in the mixture for a predetermined period of time, followed by rinsing with water. The heating temperature is set, for example, in the range of 100° C. or higher and 320° C. or lower, and the treatment time is set, for example, in the range of 1 minute or higher and 60 minutes or lower, appropriately taking into consideration the shape and size of the desired recess 7, etc. By the above-mentioned acid treatment, the inorganic particles on the surface of the sintered body 11 and the spaces between the phosphor particles 17 are preferentially dissolved, and the sintered body 11 is regranulated. The gaps are preferentially dissolved and return to a particle state. Then, the phosphor particles 17 are released and the recesses 7 are formed on the surface of the sintered body 11.
For example, when the sintered body 11 containing the phosphor particles 17 made of YAG and inorganic particles made of aluminum oxide is subjected to an acid treatment using a mixture of phosphoric acid and sulfuric acid in a ratio of 36:74, the YAG is heated to 200° C. On the other hand, aluminum oxide starts to dissolve at about 260° C., so the temperature of the mixed liquid is set in the range of 280° C. to 305° C., for example. In this way, YAG dissolves faster than aluminum oxide. Since the ratio is high, the surface of the phosphor particle 17 is preferentially dissolved between the inorganic particle and the phosphor particle 17, and the inorganic particle and the phosphor particle 17 are separated, and the phosphor particle 17 is released. A recess 7 is formed on the surface of the sintered body 11 .

このようにして、焼結体11の光反射面4には、複数の凹部7が形成される。そして、上記の酸処理をされた焼結体11では、光反射面4における蛍光体粒子17の分布は、焼結体11の内部における蛍光体粒子17の分布より少なくなる。
焼結体11単体の場合には、光反射面4における蛍光体粒子17の分布は、光反射面4を観察したSEM画像を画像解析することにより、光反射面4の面積に対する蛍光体粒子17の面積の比率として求めることができる。そして、焼結体11の内部における蛍光体粒子17の分布は、焼結体11の中心軸を含む焼結体11の断面のSEM画像を画像解析することにより、焼結体11の断面の面積に対する蛍光体粒子17の面積の比率として求めることができる。
一方で、焼結体11と反射部材21とを含む波長変換部材1の場合など、光反射面4を直接SEM画像で観察することが困難な場合には、以下の方法で求めることができる。光反射面4における蛍光体粒子17の分布は、例えば、図3Hに模式的に示す光反射面4を横断する焼結体11の断面のSEM画像を画像解析することにより、光反射面4をなぞる線L4の長さに対する、当該光反射面4の線L4において蛍光体粒子17が重なる部分の長さとの比率として求めることができる。そして、焼結体11の内部における蛍光体粒子17の分布は、焼結体11の中心軸を含む焼結体11の断面のSEM画像において、光反射面4をなぞる線L4に対応する仮想線L40を引いたものを画像解析することにより、仮想線L40の長さに対する、当該仮想線L40において蛍光体粒子17が重なる部分の長さとの比率として求めることができる。ここで、図3Hは画像解析する範囲の一部を拡大して示すものであり、実際に分布を求める際のSEM画像において画像解析する範囲は、解析位置により分布が異なることがないよう一定以上の範囲、例えば、蛍光体粒子17が100個映るスケールに設定することは言うまでもない。光反射面4における蛍光体粒子17の分布は、例えば、焼結体11の内部における蛍光体粒子17の分布の0.3倍以下、好ましくは0.1倍以下、さらに好ましくは、ほぼ0である。このような蛍光体粒子分布とすることにより、焼結体11の光反射面4には無機物粒子がより多く分布するため、焼結体11の光反射面4における光の閉じ込めを向上させることができる。これは、無機物粒子と凹部7の空隙9との間の屈折率差によるものと考えられる。また、焼結体11の光反射面4に露出する蛍光体粒子17が減少することによるものとも考えられる。なお、図3Hは、蛍光体粒子17の分布を評価する方法を説明するための簡略化した模式図であり、断面図であるが線L4及び仮想線L40を把握しやすいようにハッチングは省略している。また、図3Hにおいて、蛍光体粒子17を同一の直径の円形に描いているが、実際は個々の蛍光体粒子17の粒径及び形状は異なっている。
In this way, a plurality of recesses 7 are formed on the light reflecting surface 4 of the sintered body 11. In the sintered body 11 that has been subjected to the above-mentioned acid treatment, the distribution of the phosphor particles 17 on the light reflecting surface 4 is smaller than the distribution of the phosphor particles 17 inside the sintered body 11.
In the case of the sintered body 11 alone, the distribution of the phosphor particles 17 on the light reflecting surface 4 can be found as the ratio of the area of the phosphor particles 17 to the area of the light reflecting surface 4 by performing image analysis on an SEM image of the light reflecting surface 4. The distribution of the phosphor particles 17 inside the sintered body 11 can be found as the ratio of the area of the phosphor particles 17 to the area of the cross section of the sintered body 11 by performing image analysis on an SEM image of a cross section of the sintered body 11 including the central axis of the sintered body 11.
On the other hand, in the case of a wavelength conversion member 1 including a sintered body 11 and a reflecting member 21, when it is difficult to directly observe the light reflecting surface 4 in an SEM image, the distribution of the phosphor particles 17 on the light reflecting surface 4 can be obtained by, for example, image analysis of an SEM image of a cross section of the sintered body 11 crossing the light reflecting surface 4 as shown in FIG. 3H, as a ratio of the length of the portion where the phosphor particles 17 overlap on the line L4 of the light reflecting surface 4 to the length of the line L4 of the light reflecting surface 4. The distribution of the phosphor particles 17 inside the sintered body 11 can be obtained by image analysis of an SEM image of a cross section of the sintered body 11 including the central axis of the sintered body 11, by drawing a virtual line L40 corresponding to the line L4 tracing the light reflecting surface 4, as a ratio of the length of the portion where the phosphor particles 17 overlap on the virtual line L40 to the length of the virtual line L40. Here, FIG. 3H shows an enlarged view of a portion of the range to be image-analyzed, and it goes without saying that the range to be image-analyzed in the SEM image when actually obtaining the distribution is set to a certain range or more, for example, a scale in which 100 phosphor particles 17 are reflected, so that the distribution does not differ depending on the analysis position. The distribution of the phosphor particles 17 on the light-reflecting surface 4 is, for example, 0.3 times or less, preferably 0.1 times or less, and more preferably, approximately 0, of the distribution of the phosphor particles 17 inside the sintered body 11. By making such a phosphor particle distribution, more inorganic particles are distributed on the light-reflecting surface 4 of the sintered body 11, so that the confinement of light on the light-reflecting surface 4 of the sintered body 11 can be improved. This is considered to be due to the difference in refractive index between the inorganic particles and the voids 9 of the recesses 7. It is also considered to be due to the reduction in the phosphor particles 17 exposed on the light-reflecting surface 4 of the sintered body 11. Note that FIG. 3H is a simplified schematic diagram for explaining a method for evaluating the distribution of the phosphor particles 17, and although it is a cross-sectional view, hatching is omitted to make it easier to understand the line L4 and the virtual line L40. In addition, in FIG. 3H, the phosphor particles 17 are drawn as circles having the same diameter, but in reality, the particle size and shape of each phosphor particle 17 are different.

言い換えれば、焼結体11において、光反射面4を含む周縁領域111における蛍光体粒子17の分布が、当該周縁領域111より内側の内部領域112における蛍光体粒子17の分布よりも小さくなる。ここで、焼結体11の光反射面4を含む周縁領域111とは、焼結体11の光反射面4から内側に一定の距離の領域を指す。一定の距離とは、酸処理の温度や時間等の条件にもよるが、例えば、5μm以上、20μm以下をいう。焼結体11の光反射面4を含む周縁領域111における蛍光体粒子17の密度は、内部領域112における蛍光体粒子17の密度の、例えば、0.3倍以下、好ましくは0.1倍以下、さらに好ましくは、密度がほぼ0である。このような蛍光体粒子分布とすることにより、焼結体11の光反射面4を含む周縁領域111には無機物粒子がより多く分布するため、焼結体11の光反射面4における光の閉じ込めを向上させることができる。これは、無機物粒子と凹部7の空隙9との間の屈折率差によるものと考えられる。また、焼結体11の光反射面4に露出する蛍光体粒子17が減少することによるものとも考えられる。また、これにより、焼結体11に光を照射したときの、焼結体11の周縁領域111と内部領域112における色ムラを低減することができる。 In other words, in the sintered body 11, the distribution of the phosphor particles 17 in the peripheral region 111 including the light reflecting surface 4 is smaller than the distribution of the phosphor particles 17 in the internal region 112 inside the peripheral region 111. Here, the peripheral region 111 including the light reflecting surface 4 of the sintered body 11 refers to a region at a certain distance inward from the light reflecting surface 4 of the sintered body 11. The certain distance depends on the conditions such as the temperature and time of the acid treatment, but is, for example, 5 μm or more and 20 μm or less. The density of the phosphor particles 17 in the peripheral region 111 including the light reflecting surface 4 of the sintered body 11 is, for example, 0.3 times or less, preferably 0.1 times or less, and more preferably, the density is almost 0, of the density of the phosphor particles 17 in the internal region 112. By making such a phosphor particle distribution, more inorganic particles are distributed in the peripheral region 111 including the light reflecting surface 4 of the sintered body 11, so that the confinement of light in the light reflecting surface 4 of the sintered body 11 can be improved. This is believed to be due to the difference in refractive index between the inorganic particles and the voids 9 in the recesses 7. It is also believed to be due to a decrease in the phosphor particles 17 exposed to the light reflecting surface 4 of the sintered body 11. This also reduces color unevenness in the peripheral region 111 and the internal region 112 of the sintered body 11 when the sintered body 11 is irradiated with light.

また、上記酸処理によって、焼結体11から蛍光体粒子17が離脱することにより、焼結体11の光反射面4を含む周縁領域111において、焼結体11に囲まれた空隙9を形成することができる。これにより、焼結体11の光反射面4での光の閉じ込めをさらに高くすることができる。ここで、焼結体11に囲まれるとは、焼結体11の一断面において、空隙9の外周の40%以上、80%以下に焼結体11があることをいう。
焼結体11の光反射面4を含む周縁領域111における空隙率は、5%以上、30%以下とすることが好ましい。これにより、焼結体11の強度を保ちつつ、光反射面4における光の閉じ込めを向上させることができる。
Furthermore, the acid treatment causes the phosphor particles 17 to separate from the sintered body 11, thereby forming voids 9 surrounded by the sintered body 11 in the peripheral region 111 including the light reflecting surface 4 of the sintered body 11. This further enhances the confinement of light at the light reflecting surface 4 of the sintered body 11. Here, being surrounded by the sintered body 11 means that the sintered body 11 is present in 40% or more and 80% or less of the periphery of the voids 9 in one cross section of the sintered body 11.
The porosity of the peripheral region 111 including the light reflecting surface 4 of the sintered body 11 is preferably 5% or more and 30% or less. This makes it possible to improve the confinement of light at the light reflecting surface 4 while maintaining the strength of the sintered body 11.

3.反射部材配置工程S3
ここでは、表面に凹部7が形成された柱形状の焼結体11の外周側面に接して外周側面を取り囲む反射部材21を配置する。ここで、焼結体11の外周側面は光反射面4である。
例えば、反射部材21を形成する反射部材用粉体を、所定の位置に配置した柱形状の焼結体11を取り囲むように一体的に成形して焼結させる。反射部材21を形成する反射部材用粉体の成形は、例えば、スリップキャスト法、ドクターブレード法等により、所定の位置に配置した焼結体11を取り囲むように成形する。この成形の際、または成形後に圧力をかけてより緻密に充填するようにしてもよい。これにより、柱形状の焼結体11と反射部材21とが一体化された波長変換部材1が作製される。なお、反射部材21を形成する反射部材用粉体を焼結させる際、焼結体11はあらかじめ焼結させているので、反射部材21と一体化された後においても表面に形成された凹部7を含め柱形状の焼結体11の形状は実質的に変形することなく維持される。反射部材21を配置した後、反射部材21で覆われた焼結体11の光反射面4以外の表面、言い換えると、反射部材から露出される表面の一部または全部を必要に応じて研削または研磨することにより該表面に形成された凹部7を除去することができる。
3. Reflective member arrangement step S3
Here, a reflecting member 21 is disposed in contact with and surrounding the outer peripheral side surface of a columnar sintered body 11 having a recess 7 formed on its surface. The outer peripheral side surface of the sintered body 11 is a light reflecting surface 4.
For example, the powder for the reflecting member forming the reflecting member 21 is molded and sintered integrally so as to surround the columnar sintered body 11 arranged at a predetermined position. The powder for the reflecting member forming the reflecting member 21 is molded, for example, by a slip cast method, a doctor blade method, or the like so as to surround the sintered body 11 arranged at a predetermined position. Pressure may be applied during or after this molding to pack more densely. This produces a wavelength conversion member 1 in which the columnar sintered body 11 and the reflecting member 21 are integrated. Note that when the powder for the reflecting member forming the reflecting member 21 is sintered, the sintered body 11 is sintered in advance, so that the shape of the columnar sintered body 11 including the recesses 7 formed on the surface is maintained without substantial deformation even after integration with the reflecting member 21. After the reflecting member 21 is arranged, the surface other than the light reflecting surface 4 of the sintered body 11 covered with the reflecting member 21, in other words, a part or all of the surface exposed from the reflecting member, can be ground or polished as necessary to remove the recesses 7 formed on the surface.

反射部材21は、焼結体11の無機物粒子と同じ材料を含んで構成することが好ましく、例えば、酸化アルミニウムを主原料として含み、酸化アルミニウムとは異なる屈折率の材料も含むものを用いることができる。
ここで、例えば、スリップキャスト法、ドクターブレード法等により反射部材用粉体を成形する場合、焼結体11の凹部7の一部または全部に反射部材用粉体が侵入することがある。この場合、焼結体11の光反射面4と反射部材21aの境界では、焼結体11の凹部7と、凹部7内に延在する反射部材21aの凸部8の少なくとも一部と、凹部7と凸部8との間に形成される空隙9と、を含む中間領域が形成される。ここで、中間領域とは、酸処理の温度や時間等の条件にもよるが、例えば、焼結体11の光反射面4と、反射部材21aの境界から、焼結体11側及び反射部材21a側それぞれに一定の距離の領域を指す。一定の距離とは、酸処理の温度や時間等の条件にもよるが、例えば、3μm以上、10μm以下の領域をいう。
なお、焼結体11の凹部7と、反射部材21aの凸部8と、凹部7と凸部8との間に形成される空隙9については模式的に示した図には図示していないが、図7A及び図7Bに示す。
The reflecting member 21 is preferably made of the same material as the inorganic particles of the sintered body 11, and for example, a material containing aluminum oxide as a main raw material and also containing a material with a refractive index different from that of aluminum oxide can be used.
Here, for example, when the powder for the reflecting member is molded by the slip casting method, the doctor blade method, or the like, the powder for the reflecting member may penetrate into a part or all of the recessed portion 7 of the sintered body 11. In this case, at the boundary between the light reflecting surface 4 of the sintered body 11 and the reflecting member 21a, an intermediate region is formed, which includes the recessed portion 7 of the sintered body 11, at least a part of the protruding portion 8 of the reflecting member 21a extending into the recessed portion 7, and the gap 9 formed between the recessed portion 7 and the protruding portion 8. Here, the intermediate region refers to, for example, a region at a certain distance from the boundary between the light reflecting surface 4 of the sintered body 11 and the reflecting member 21a on the sintered body 11 side and the reflecting member 21a side, depending on the conditions such as the temperature and time of the acid treatment. The certain distance refers to, for example, a region of 3 μm or more and 10 μm or less, depending on the conditions such as the temperature and time of the acid treatment.
It should be noted that the recess 7 of the sintered body 11, the protrusion 8 of the reflecting member 21a, and the gap 9 formed between the recess 7 and the protrusion 8 are not shown in the schematic diagram, but are shown in Figures 7A and 7B.

ここで、反射部材配置工程S3では、図3Cから図3Fに示すように、複数の波長変換部材1が一括して作製された波長変換部材集合体を作製してもよい。その後、該波長変換部材集合体を分割して複数の波長変換部材1を作製する個片化工程を含んでいてもよい。分割後の波長変換部材1はそれぞれ、1又は2以上の焼結体11aを含んでいる。具体的には、図3Cに示す波長変換部材集合体を所定の厚さに加工することで、図3D及び図3Eに示す、複数の波長変換部材1を含む波長変換部材集合体を複数形成し、さらにその波長変換部材集合体を個々の波長変換部材1に分割するようにして、図3Fに示す波長変換部材1を得てもよい。このように波長変換部材集合体を所定の厚さに加工して、さらに個片化するようにすると、波長変換部材1の加工面に露出した焼結体11aの表面は凹部7が除去されて光の閉じ込めが抑えられることになり、別途凹部7を除去する工程を経ることなく、例えば、光入射面5または光出射面6として利用できる。また、波長変換部材集合体が所定の厚さに加工されているため、波長変換部材1が2以上の焼結体11aを含む場合、2以上の焼結体11aの光入射面及び/又は光出射面は略同一面上に位置する。 Here, in the reflecting member arrangement step S3, as shown in Figures 3C to 3F, a wavelength conversion member assembly in which multiple wavelength conversion members 1 are produced at once may be produced. After that, a singulation step may be included in which the wavelength conversion member assembly is divided to produce multiple wavelength conversion members 1. Each wavelength conversion member 1 after the division includes one or more sintered bodies 11a. Specifically, by processing the wavelength conversion member assembly shown in Figure 3C to a predetermined thickness, multiple wavelength conversion member assemblies including multiple wavelength conversion members 1 shown in Figures 3D and 3E may be formed, and the wavelength conversion member assembly may be further divided into individual wavelength conversion members 1 to obtain the wavelength conversion member 1 shown in Figure 3F. In this way, when the wavelength conversion member assembly is processed to a predetermined thickness and further singulated, the surface of the sintered body 11a exposed on the processed surface of the wavelength conversion member 1 has the recess 7 removed, suppressing light confinement, and can be used, for example, as the light incident surface 5 or the light exit surface 6 without undergoing a separate step of removing the recess 7. In addition, since the wavelength conversion member assembly is processed to a predetermined thickness, when the wavelength conversion member 1 includes two or more sintered bodies 11a, the light entrance surface and/or light exit surface of the two or more sintered bodies 11a are located on approximately the same plane.

以上のようにして作製された波長変換部材1は、焼結体11aと反射部材21aを含み、焼結体11aの側面が反射部材21aによって覆われ、焼結体11aの上面及び下面が反射部材21aから露出されている。換言すると、反射部材21aの内周側面の一部が焼結体11aの外周側面に接し、焼結体11aの光入射面及び光出射面が反射部材21aから露出している。これにより、例えば、図3Gに示すように、焼結体11aの下面を光入射面5として例えばレーザダイオード等の発光素子80の光を入射させ、上面を光出射面6として波長変換後の光を出射させることができる。このように焼結体11aの下面を光入射面5とし、上面を光出射面6とする場合、上記光入射面5及び光出射面6における光の閉じ込めを抑えるために、凹部形成工程S2後に、光入射面5及び/又は光出射面6の凹部7を除去する凹部除去工程を含むことが好ましい。実施形態1では、上述の加工により波長変換部材1を形成する工程が凹部除去工程を兼ねている。 The wavelength conversion member 1 produced as described above includes a sintered body 11a and a reflecting member 21a, the side of the sintered body 11a is covered by the reflecting member 21a, and the upper and lower surfaces of the sintered body 11a are exposed from the reflecting member 21a. In other words, a part of the inner peripheral side surface of the reflecting member 21a contacts the outer peripheral side surface of the sintered body 11a, and the light incident surface and light exit surface of the sintered body 11a are exposed from the reflecting member 21a. As a result, for example, as shown in FIG. 3G, the lower surface of the sintered body 11a can be used as the light incident surface 5 to allow light from a light emitting element 80 such as a laser diode to enter, and the upper surface can be used as the light exit surface 6 to allow light after wavelength conversion to exit. In this way, when the lower surface of the sintered body 11a is used as the light incident surface 5 and the upper surface is used as the light exit surface 6, in order to suppress light confinement in the light incident surface 5 and the light exit surface 6, it is preferable to include a recess removal step of removing the recess 7 of the light incident surface 5 and/or the light exit surface 6 after the recess formation step S2. In the first embodiment, the process of forming the wavelength conversion member 1 by the above-mentioned processing also serves as the recess removal process.

また、以上のように構成された波長変換部材1において、焼結体11aの光反射面4は複数の凹部7を有し、焼結体11aの光反射面4に対向する反射部材21aの面は、複数の凸部8を有している。そして、焼結体11aの光反射面4に形成された凹部7内に反射部材21aの凸部8の少なくとも一部が入り込み、さらに、少なくとも一部の凹部7内には空隙9も存在する。すなわち、焼結体11aの光反射面4とそれに対向する反射部材21aの面の境界には、複数の凹部7、複数の凸部8及び空隙9が存在する中間領域が形成される。この中間領域が形成されることにより、焼結体11aの凹部7を形成する無機物粒子または空隙9と、反射部材21aの凸部8との界面により、焼結体11aからの光の伝搬を抑制することで、焼結体11aの光出射面6と、光出射面6の外側とで、上面から観察した際の輝度差を大きくすることができる。また、焼結体11aの下面を光入射面5とし、上面を光出射面6とする場合、焼結体11aの光入射面5にDBR(Distributed Bragg Reflector)膜等の光学薄膜を形成するようにしてもよい。 In addition, in the wavelength conversion member 1 configured as described above, the light reflecting surface 4 of the sintered body 11a has a plurality of recesses 7, and the surface of the reflecting member 21a facing the light reflecting surface 4 of the sintered body 11a has a plurality of protrusions 8. At least a portion of the protrusions 8 of the reflecting member 21a enters into the recesses 7 formed on the light reflecting surface 4 of the sintered body 11a, and at least a portion of the recesses 7 also has voids 9. That is, an intermediate region in which a plurality of recesses 7, a plurality of protrusions 8, and voids 9 exist is formed at the boundary between the light reflecting surface 4 of the sintered body 11a and the surface of the reflecting member 21a facing it. By forming this intermediate region, the inorganic particles or voids 9 forming the recesses 7 of the sintered body 11a and the interface between the protrusions 8 of the reflecting member 21a suppress the propagation of light from the sintered body 11a, thereby increasing the luminance difference between the light exit surface 6 of the sintered body 11a and the outside of the light exit surface 6 when observed from above. Furthermore, if the lower surface of the sintered body 11a is the light incident surface 5 and the upper surface is the light exit surface 6, an optical thin film such as a DBR (Distributed Bragg Reflector) film may be formed on the light incident surface 5 of the sintered body 11a.

上記工程を経て作製された波長変換部材1では、反射部材21aによって覆われた焼結体11aの光反射面4は、酸処理により複数の凹部7が形成されているため光の閉じ込めが向上している。これにより、反射部材21aによって回りが囲まれた焼結体11aの上面を光出射面6としたときに、該光出射面6と該光出射面6の近傍の反射部材21aとの間の輝度差を大きく、言い換えれば、波長変換部材1の上面(焼結体11aの光出射面6を含む面)において、光出射面6からの離間距離に対する輝度の減少率を急峻にでき見切りを良好にできる。 In the wavelength conversion member 1 produced through the above process, the light reflecting surface 4 of the sintered body 11a covered with the reflecting member 21a has multiple recesses 7 formed by acid treatment, improving light confinement. As a result, when the upper surface of the sintered body 11a surrounded by the reflecting member 21a is used as the light emitting surface 6, the luminance difference between the light emitting surface 6 and the reflecting member 21a in the vicinity of the light emitting surface 6 is large; in other words, the rate of decrease in luminance with respect to the distance from the light emitting surface 6 on the upper surface of the wavelength conversion member 1 (the surface including the light emitting surface 6 of the sintered body 11a) can be made steep, resulting in good visibility.

以上のようにして作製された波長変換部材1は、例えば、発光ダイオードまたは半導体レーザ素子を収納するパッケージの蓋体または蓋体の一部として使用され、パッケージ内に収納された発光ダイオードまたは半導体レーザ素子からの光を波長変換して出射させることができる。 The wavelength conversion member 1 produced in the above manner can be used, for example, as a lid or part of a lid for a package that houses a light-emitting diode or a semiconductor laser element, and can convert the wavelength of light from the light-emitting diode or semiconductor laser element housed in the package and emit it.

実施形態2.
実施形態2の波長変換部材2の製造方法は、実施形態1の波長変換部材1の製造方法と同様、焼結体準備工程S1と、凹部形成工程S2と、反射部材配置工程S3とを含むものであるが、各工程の具体的内容は実施形態1とは一部異なっている。
以下、実施形態2の波長変換部材2の製造方法について詳細に説明する。
Embodiment 2.
The method for producing the wavelength conversion member 2 of embodiment 2 is similar to the method for producing the wavelength conversion member 1 of embodiment 1, and includes a sintered body preparation step S1, a recess formation step S2, and a reflective member arrangement step S3, but the specific content of each step is partially different from embodiment 1.
A method for producing the wavelength conversion member 2 of the second embodiment will be described in detail below.

1.焼結体準備工程S1
焼結体準備工程S1は、実施形態1と同様、図2に示す、(1-1)秤量工程S11と、(1-2)混合工程S12と、(1-3)成形工程S13と、(1-4)焼結工程S14と、(1-5)加工工程S15と、を含む。
実施形態2において、(1-1)秤量工程S11と(1-2)混合工程S12は、実施形態1と同様である。
そして、実施形態2では、秤量混合した無機物粒子及び蛍光体粒子を用いて、(1-3)成形工程S13において所定の厚さの板状成形体を成形する。
実施形態2において、例えば、成形工程S13では、無機物粒子と蛍光体粒子の混合粉体に、例えば、樹脂からなるバインダーと溶剤とを加えて撹拌してスラリーを作製する。そして、そのスラリーを所定の厚さに成膜した後、所定の形状に切断して板状グリーン成形体を作製する。なお、実施形態2の成形工程では、実施形態1と同様にして、プレス成型及び/又はCIP(冷間静水圧加圧)成形等により板状に成形するようにしてもよい。
なお、板状成形体の厚さは、後述の焼結による収縮を考慮して、焼結後の厚さが所望の厚さになるように設定する。
1. Sintered body preparation step S1
The sintered body preparation step S1 includes, as in the first embodiment, (1-1) a weighing step S11, (1-2) a mixing step S12, (1-3) a molding step S13, (1-4) a sintering step S14, and (1-5) a processing step S15, as shown in FIG.
In the second embodiment, the (1-1) weighing step S11 and the (1-2) mixing step S12 are the same as those in the first embodiment.
In the second embodiment, the weighed and mixed inorganic particles and phosphor particles are used to form a plate-shaped molded body having a predetermined thickness in the (1-3) molding step S13.
In the second embodiment, for example, in the molding step S13, a binder made of resin and a solvent are added to the mixed powder of inorganic particles and phosphor particles, and the mixture is stirred to prepare a slurry. The slurry is then formed into a film of a predetermined thickness, and then cut into a predetermined shape to prepare a plate-shaped green compact. In the molding step of the second embodiment, the green compact may be molded into a plate shape by press molding and/or CIP (cold isostatic pressing) molding, etc., in the same manner as in the first embodiment.
The thickness of the plate-like molded body is set so that the thickness after sintering will be a desired thickness, taking into consideration the shrinkage due to sintering described below.

次に、(1-4)焼結工程S14において、実施形態1と同様にして、板状成形体を焼結することにより、焼結体である蛍光体セラミック板12を作製する。 Next, in the sintering step (1-4) S14, the plate-shaped molded body is sintered in the same manner as in embodiment 1 to produce a sintered body, the phosphor ceramic plate 12.

(1-5)加工工程S15
得られた蛍光体セラミック板12の上面に図4Aに示すように、円錐台形状の複数の凸部12aを形成する。この凸部12aは、例えば、マシニングセンター等により形成することができる。なお、蛍光体セラミック板12において、複数の凸部12aを除いた部分をベース部12bという。
(1-5) Processing process S15
As shown in Fig. 4A, a plurality of convex portions 12a having a truncated cone shape are formed on the upper surface of the obtained phosphor ceramic plate 12. The convex portions 12a can be formed, for example, by a machining center or the like. The portion of the phosphor ceramic plate 12 excluding the plurality of protrusions 12 a is referred to as a base portion 12 b.

2.凹部形成工程S2
実施形態2において、凹部形成工程S2は、
(i)蛍光体セラミック板12全体を酸処理して蛍光体セラミック板12の表面全体に凹部7を形成する酸処理工程と、
(ii)所定の面の凹部7を除去した後、所定の形状の焼結体12aに分離する第2加工工程と、
を含む。
2. Recess formation step S2
In embodiment 2, the recess forming step S2 includes:
(i) an acid treatment step in which the entire phosphor ceramic plate 12 is subjected to an acid treatment to form recesses 7 on the entire surface of the phosphor ceramic plate 12;
(ii) a second processing step of removing the recesses 7 on the predetermined surface and then separating the sintered body 12a into a predetermined shape;
Includes.

(2-1)酸処理工程
実施形態2の凹部形成工程S2において、酸処理工程では、複数の凸部12aが形成された蛍光体セラミック板12全体を酸処理し、図4Bに示すように、複数の凸部12aの表面を含む蛍光体セラミック板12全体の表面に複数の凹部7を形成する。酸処理は、実施形態1と同様に行う。
In the acid treatment step S2 of the recess formation step of the second embodiment, the entire phosphor ceramic plate 12 on which the plurality of protrusions 12a are formed is subjected to an acid treatment to form a plurality of recesses 7 on the entire surface of the phosphor ceramic plate 12 including the surfaces of the plurality of protrusions 12a, as shown in Fig. 4B. The acid treatment is performed in the same manner as in the first embodiment.

(2-2)第2加工工程
第2加工工程では、まず、円錐台形状の複数の凸部12aの上面をそれぞれ研削して、該上面に形成された凹部7を除去し、図4Cに示すように、上面を平坦にする。
次に、蛍光体セラミック板12の下面からベース部12bを研削することにより、ベース部12bを除去して、図4Dに示すように、円錐台形状の複数の凸部12aを個々に分離する。
以上のようにして、上底面及び下底面がそれぞれ平坦で外周側面に酸処理による凹部7が形成された、円錐台形状の焼結体12aを作製する。
ここで、本明細書において、円錐台形状の上底または上底面とは、上下の位置関係にかかわらず、側面を挟んで対向する円形の面のうちの面積の小さい面をいい、当該対向する円形の面のうちの面積の大きい面を下底または下底面という。
(2-2) Second Processing Step In the second processing step, first, the upper surfaces of the multiple truncated cone-shaped protrusions 12a are ground to remove the recesses 7 formed on the upper surfaces, and the upper surfaces are made flat as shown in FIG. 4C.
Next, the base portion 12b is removed by grinding from the lower surface of the phosphor ceramic plate 12, and the plurality of truncated cone-shaped protrusions 12a are separated into individual pieces as shown in FIG. 4D.
In this manner, a sintered body 12a having a truncated cone shape is produced, the upper and lower bottom surfaces of which are flat, and the recesses 7 formed on the outer peripheral side surface by acid treatment.
In this specification, the upper base or upper base surface of the truncated cone shape refers to the smaller area of the circular surfaces facing each other across the side surface, regardless of the vertical positional relationship, and the larger area of the opposing circular surfaces is referred to as the lower base or lower base surface.

3.反射部材配置工程S3
ここでは、表面に凹部7が形成された柱形状の焼結体12aの外周側面に接して外周側面を取り囲む反射部材22を配置する。ここで、焼結体12aの外周側面は光反射面4である。
具体的には、まず、円錐台形状の焼結体12aが内部に挿入される貫通孔が形成された反射部材22を別途作製する。例えば、反射部材22を形成する反射部材用粉体を、成形して貫通孔を含む成形体を作製し、その成形体を焼結することにより反射部材22を作製する。焼結後、貫通孔を研削または研磨加工して所定の寸法精度に仕上げるようにしてもよい。このようにすると貫通孔内に円錐台形状の焼結体12aを高い位置精度で配置することができる。反射部材22の貫通孔は、焼結体12aと同じ円錐台形状であり、上底の開口面が焼結体12aの上底より小さく、下底の開口面が焼結体12aの下底より大きくなるように形成される。実施形態2では、反射部材22としてセラミックを用いているが、例えば、メタルを用いることもできる。
ここで、焼結体12aを反射部材22の貫通孔内に配置する前に、貫通孔の内壁に低融点ガラスを形成することができる。そして、焼結体12aを反射部材22の貫通孔内に低融点ガラスを用いて融着することで、焼結体12aを反射部材22の貫通孔内に固定することができる。これにより、反射部材22の貫通孔の傾斜角と、焼結体12aの側面の傾斜角とを同一にしなくても、焼結体12aからの放熱性や、固定強度を向上させる事ができる。なお、反射部材22の貫通孔の傾斜角と、焼結体12aの側面の傾斜角とを同一にしてもよい。
3. Reflective member arrangement step S3
Here, a reflecting member 22 is disposed in contact with and surrounding the outer peripheral side surface of a columnar sintered body 12a having a recess 7 formed on its surface. The outer peripheral side surface of the sintered body 12a is the light reflecting surface 4.
Specifically, first, the reflecting member 22 is separately prepared, in which a through hole is formed and the sintered body 12a having a truncated cone shape is inserted therein. For example, the powder for the reflecting member forming the reflecting member 22 is molded to prepare a molded body having a through hole, and the molded body is sintered to prepare the reflecting member 22. After sintering, the through hole may be ground or polished to a predetermined dimensional accuracy. In this way, the sintered body 12a having a truncated cone shape can be placed in the through hole with high positional accuracy. The through hole of the reflecting member 22 has the same truncated cone shape as the sintered body 12a, and is formed so that the opening surface of the upper base is smaller than the upper base of the sintered body 12a and the opening surface of the lower base is larger than the lower base of the sintered body 12a. In the second embodiment, ceramic is used as the reflecting member 22, but for example, metal can also be used.
Here, before placing the sintered body 12a in the through hole of the reflecting member 22, low melting point glass can be formed on the inner wall of the through hole. Then, the sintered body 12a can be fused into the through hole of the reflecting member 22 using the low melting point glass, thereby fixing the sintered body 12a in the through hole of the reflecting member 22. This makes it possible to improve the heat dissipation from the sintered body 12a and the fixing strength even if the inclination angle of the through hole of the reflecting member 22 and the inclination angle of the side surface of the sintered body 12a are not the same. Note that the inclination angle of the through hole of the reflecting member 22 and the inclination angle of the side surface of the sintered body 12a may be the same.

次に、図4Fに示すように、反射部材22の貫通孔に円錐台形状の焼結体12aを挿入する。上述したように、貫通孔は上底の開口面が焼結体12aの上底より小さく、下底の開口面が焼結体12aの下底より大きくなるように形成されているので、図4Fに示すように、焼結体12aは、貫通孔の途中、すなわち、貫通孔において上底側及び下底側の双方に空洞が形成されるように貫通孔内に保持される。
次いで、図4Gに示すように、焼結体12aを挿入した貫通孔の、下底側の空洞を上にして該空洞内にガラス18を塗布して溶融させ、焼結体12aの上にガラス18を配置する。実施形態2では、ガラス18は蛍光体を含んでいるが、蛍光体を含まない構成とすることもできるし、光拡散材等を含んでいてもよい。
その後、貫通孔から突出したガラス18を研削及び/又は研磨して、図4Hに示すように、ガラス18の表面と反射部材22の上面とが同一平面を形成するようにする。
Next, as shown in Fig. 4F, the truncated cone-shaped sintered body 12a is inserted into the through-hole of the reflecting member 22. As described above, the through-hole is formed so that the opening surface of the upper base is smaller than the upper base of the sintered body 12a and the opening surface of the lower base is larger than the lower base of the sintered body 12a, so that the sintered body 12a is held in the middle of the through-hole, i.e., so that cavities are formed on both the upper and lower sides of the through-hole, as shown in Fig. 4F.
4G, the through hole into which the sintered body 12a has been inserted is placed with the bottom side of the cavity facing up, and glass 18 is applied and melted in the cavity, and the glass 18 is placed on the sintered body 12a. In the second embodiment, the glass 18 contains a phosphor, but it may be configured not to contain a phosphor, or may contain a light diffusing material or the like.
Thereafter, the glass 18 protruding from the through hole is ground and/or polished so that the surface of the glass 18 and the upper surface of the reflecting member 22 form the same plane as shown in FIG. 4H.

以上のようにして作製された実施形態2の波長変換部材2は、焼結体12aと反射部材22を含み、円錐台形状の焼結体12aの側面が反射部材22によって覆われ、焼結体12aの上面及び下面が反射部材22から露出されている。これにより、例えば、図4Iに示すように、焼結体12aの下面を光入射面5として例えばレーザダイオード等の発光素子80の光を入射させ、上面を光出射面6として波長変換後の光を出射させることができる。このように焼結体12aの下面を光入射面5とし、上面を光出射面6とする場合、当該光入射面5及び光出射面6における光の閉じ込めを抑えるために、凹部形成工程S2後に、光入射面5及び/又は光出射面6凹部7を除去する凹部除去工程を含むことが好ましい。実施形態2では、上述の第2加工工程における、凸部12aの上面を研削及び/又は研磨する工程、及びベース部12bを除去して複数の凸部12aを個々に分離する工程が、凹部除去工程を兼ねている。また、焼結体12aの下面を光入射面5とし、上面を光出射面6とする場合、焼結体12aの光入射面5に反射防止膜を形成するようにしてもよい。 The wavelength conversion member 2 of the second embodiment produced as described above includes a sintered body 12a and a reflecting member 22, and the side of the frustum-shaped sintered body 12a is covered by the reflecting member 22, and the upper and lower surfaces of the sintered body 12a are exposed from the reflecting member 22. As a result, for example, as shown in FIG. 4I, the lower surface of the sintered body 12a can be used as the light incident surface 5 to allow light from a light emitting element 80 such as a laser diode to enter, and the upper surface can be used as the light exit surface 6 to allow light after wavelength conversion to exit. In this way, when the lower surface of the sintered body 12a is used as the light incident surface 5 and the upper surface is used as the light exit surface 6, in order to suppress light confinement in the light incident surface 5 and the light exit surface 6, it is preferable to include a recess removal step of removing the recess 7 of the light incident surface 5 and/or the light exit surface 6 after the recess formation step S2. In the second embodiment, the process of grinding and/or polishing the upper surface of the convex portion 12a and the process of removing the base portion 12b to separate the multiple convex portions 12a in the second processing process described above also serve as a recess removing process. In addition, when the lower surface of the sintered body 12a is the light incident surface 5 and the upper surface is the light exit surface 6, an anti-reflection film may be formed on the light incident surface 5 of the sintered body 12a.

上記工程を経て作製された波長変換部材2では、反射部材22によって覆われた焼結体12aの光反射面4は、酸処理により複数の凹部7が形成されているため光の閉じ込めが向上している。これにより、反射部材22によって回りが囲まれた焼結体12aの上面を光出射面6としたときに、該光出射面6と該光出射面6の近傍の反射部材22との間の輝度差を大きく、言い換えれば、波長変換部材2の上面(焼結体12aの光出射面6とそれを囲む反射部材22の上面)において、光出射面6からの離間距離に対する輝度の減少率を急峻にでき見切りを良好にできる。 In the wavelength conversion member 2 produced through the above process, the light reflecting surface 4 of the sintered body 12a covered with the reflecting member 22 has multiple recesses 7 formed by acid treatment, improving light confinement. As a result, when the upper surface of the sintered body 12a surrounded by the reflecting member 22 is used as the light emitting surface 6, the luminance difference between the light emitting surface 6 and the reflecting member 22 in the vicinity of the light emitting surface 6 is large; in other words, the rate of decrease in luminance with respect to the distance from the light emitting surface 6 on the upper surface of the wavelength conversion member 2 (the light emitting surface 6 of the sintered body 12a and the upper surface of the reflecting member 22 surrounding it) can be made steep, resulting in good visibility.

以上のようにして作製された波長変換部材2は、例えば、発光ダイオードまたは半導体レーザ素子を収納するパッケージの蓋体または蓋体の一部として使用され、パッケージ内に収納された発光ダイオードまたは半導体レーザ素子からの光を波長変換して出射させることができる。 The wavelength conversion member 2 produced in the above manner can be used, for example, as a lid or part of a lid for a package that houses a light-emitting diode or semiconductor laser element, and can convert the wavelength of light from the light-emitting diode or semiconductor laser element housed in the package and emit it.

実施の形態3
実施形態3の波長変換部材3の製造方法は、実施形態1及び2の波長変換部材の製造方法と同様、図5に示すように、焼結体準備工程S1と、凹部形成工程S2とを含むものであるが、凹部形成工程S2において、焼結体13の形状加工と表面への凹部7の形成を一括して行っている点が実施形態2とは異なっている。
また、実施形態3の製造方法により作製される波長変換部材3は、上面から入射した光を波長変換した後、上面から出射させるもの、すなわち光入射面5と光出射面6が同一の面からなる。したがって、実施形態3の製造方法は、図5に示すように、実施形態1及び2の反射部材配置工程S3に代えて、焼結体13の下面に反射膜23を形成する反射膜形成工程を含んでいる。
以下、実施形態3の波長変換部材3の製造方法について詳細に説明する。
Embodiment 3
The method of manufacturing the wavelength conversion member 3 of embodiment 3, like the methods of manufacturing the wavelength conversion members of embodiments 1 and 2, includes a sintered body preparation step S1 and a recess formation step S2 as shown in FIG. 5 . However, it differs from embodiment 2 in that in the recess formation step S2, the shape processing of the sintered body 13 and the formation of the recesses 7 on the surface are carried out in a single step.
Moreover, the wavelength conversion member 3 produced by the manufacturing method of the third embodiment converts the wavelength of light incident from the upper surface and then emits the light from the upper surface, i.e., the light incident surface 5 and the light exit surface 6 are the same surface. Therefore, the manufacturing method of the third embodiment includes a reflective film forming step of forming a reflective film 23 on the lower surface of the sintered body 13, instead of the reflective member arrangement step S3 of the first and second embodiments, as shown in FIG.
A method for producing the wavelength conversion member 3 of the third embodiment will be described in detail below.

1.焼結体準備工程S1
実施形態3の波長変換部材3の製造方法では、焼結体準備工程S1において実施形態2と同様にして板状成形体を作製し、その板状成形体を焼結することにより、焼結体である蛍光体セラミック板13を作製する。
1. Sintered body preparation step S1
In the manufacturing method of the wavelength conversion member 3 of embodiment 3, in the sintered body preparation step S1, a plate-shaped body is prepared in the same manner as in embodiment 2, and the plate-shaped body is sintered to produce a sintered body, namely, a phosphor ceramic plate 13.

2.凹部形成工程S2
実施形態3の製造方法において、凹部形成工程S2は、蛍光体セラミック板13の上面を形状加工するとともに形状加工された表面に凹部7を形成する工程である。
具体的には、まず、図6Aに示すように、蛍光体セラミック板13の上面に、例えば、SiOからなり、上面視したときの平面形状が矩形のマスク53を所定の間隔で複数形成する。このとき、形状加工を施さない蛍光体セラミック板13の下面には、全面に、例えば、SiO膜からなる保護膜55を形成することができる。または、蛍光体セラミック板13の下面に保護膜55を形成せずにエッチングを行い、後の工程において、凹部7が形成された下面を研削または研磨してもよい。蛍光体セラミック板13の厚みが比較的薄い場合、凹部7が形成された下面を研削または研磨することで蛍光体セラミック板13が割れることがあるので、そのような場合には、保護膜55を形成することが好ましい。ここで、蛍光体セラミック板13の上面に形成するマスク53及び下面に形成する保護膜55は、SiOに限定されるものではなく、例えば、SiON、SiN、Al、AlON、AlN、ZrOを用いることができるが、後述の酸処理によりエッチングされないものであればよい。
2. Recess formation step S2
In the manufacturing method of the third embodiment, the recess forming step S2 is a step of shaping the upper surface of the phosphor ceramic plate 13 and forming the recesses 7 on the shaped surface.
Specifically, first, as shown in FIG. 6A, a plurality of masks 53 made of, for example, SiO 2 and having a rectangular planar shape when viewed from above are formed at predetermined intervals on the upper surface of the phosphor ceramic plate 13. At this time, a protective film 55 made of, for example, a SiO2 film can be formed on the entire lower surface of the phosphor ceramic plate 13 that is not subjected to shaping. Alternatively, etching may be performed without forming the film 55, and the lower surface on which the recesses 7 are formed may be ground or polished in a later step. Since grinding or polishing the lower surface of the phosphor ceramic plate 13 may cause the phosphor ceramic plate 13 to crack, in such a case, it is preferable to form a protective film 55 . Here, the mask 53 formed on the upper surface of the phosphor ceramic plate 13 and the protective film 55 formed on the lower surface thereof are not limited to SiO2 , but may be, for example, SiON, SiN, Al2O3 , AlON, AlN, ZrO2 can be used, but any material that is not etched by the acid treatment described below will suffice.

次に、上面にマスク53が形成され、下面に保護膜55が形成された蛍光体セラミック板13全体を酸処理する。酸処理は、実施形態1と同様、例えば、燐酸と硫酸の混合液を加熱して、その液中で所定の時間行い、その後水洗する。実施形態1で説明したように、この酸処理により、焼結体13(蛍光体セラミック板13)の表面近傍の無機物粒子と蛍光体粒子17の粒子間が優先的に溶解されて蛍光体粒子が離脱するが、例えば、酸化アルミニウム等からなる無機物粒子も燐酸と硫酸の混合液によりある温度以上では溶解される。したがって、この酸処理により、上面におけるマスク53間の蛍光体セラミックがエッチングにより除去されて、図6Cに示すように、マスク53の下部にそれぞれ凸部13aが形成され、そのエッチングにより形成された表面には複数の凹部7が形成される。例えば、平面形状が矩形のマスク53を形成して酸処理した場合には、酸処理によるエッチングは等方的であることから、マスク53の下部に形成される凸部13aはそれぞれ略四角錐台形状になるが、その略四角錐台形状の凸部13aの側面にそれぞれ複数の凹部7が形成される。ここで、蛍光体セラミック板13の上面のうち、マスク53が形成されていない領域において、例えば、ダイシングまたはレーザ等でハーフカットを施してからエッチングをすることで、酸をさらに浸透させやすくすることができる。これにより、ハーフカットしない場合と比較して、より深くエッチングをすることができる。この結果、蛍光体セラミック板13内の光の伝搬をより抑制することができるため、見切りを向上させることができる。
なお、略四角錐台形状の凸部13aの上面、すなわちマスク53に接する面、及びマスク53の上面はそれぞれ実質的に平坦であり、蛍光体セラミック板13の光入出射面に好適である。
Next, the phosphor ceramic plate 13 having the mask 53 formed on the upper surface and the protective film 55 formed on the lower surface is subjected to an acid treatment. The acid treatment is performed in the same manner as in the first embodiment, for example, by heating a mixture of phosphoric acid and sulfuric acid, and performing the acid treatment for a predetermined time in the mixture, and then washing with water. As described in the first embodiment, this acid treatment preferentially dissolves the inorganic particles near the surface of the sintered body 13 (phosphor ceramic plate 13) and the phosphor particles 17 between the particles, and the phosphor particles are released, but inorganic particles made of, for example, aluminum oxide are also dissolved by the mixture of phosphoric acid and sulfuric acid at a certain temperature or higher. Therefore, the phosphor ceramic between the masks 53 on the upper surface is removed by etching, and as shown in FIG. 6C, convex portions 13a are formed at the lower portions of the masks 53, and a plurality of concave portions 7 are formed on the surface formed by the etching. For example, when a mask 53 having a rectangular planar shape is formed and acid treatment is performed, the etching by the acid treatment is isotropic, so that the convex portions 13a formed on the lower part of the mask 53 are each approximately quadrangular pyramid shaped, and a plurality of concave portions 7 are formed on the side surfaces of the approximately quadrangular pyramid shaped convex portions 13a. Here, in the region of the upper surface of the phosphor ceramic plate 13 where the mask 53 is not formed, for example, half-cutting is performed by dicing or laser, etc., and then etching is performed, so that the acid can be more easily penetrated. This allows etching to be performed deeper than when the half-cutting is not performed. As a result, the propagation of light in the phosphor ceramic plate 13 can be further suppressed, and the parting can be improved.
The upper surface of the approximately quadrangular pyramid-shaped protrusion 13 a , that is, the surface in contact with the mask 53 , and the upper surface of the mask 53 are both substantially flat, which is suitable for the light incident and exit surfaces of the phosphor ceramic plate 13 .

実施形態3の酸処理における、燐酸と硫酸の割合、混合液の加熱温度、処理時間等は、実施形態1等と同様にして所望の凹部7が形成されるように設定されるが、実施形態3の酸処理では、蛍光体セラミック板13の上面の形状加工も兼ねるので、形成すべき凸部13aの形状をさらに考慮して燐酸と硫酸の割合、混合液の加熱温度、処理時間等を調整するようにしてもよい。 In the acid treatment of embodiment 3, the ratio of phosphoric acid to sulfuric acid, the heating temperature of the mixed solution, the treatment time, etc. are set so that the desired recesses 7 are formed in the same manner as in embodiment 1, etc., but since the acid treatment of embodiment 3 also serves to shape the upper surface of the phosphor ceramic plate 13, the ratio of phosphoric acid to sulfuric acid, the heating temperature of the mixed solution, the treatment time, etc. may be adjusted taking into further consideration the shape of the protrusions 13a to be formed.

3.反射膜形成工程
酸処理後、図6Dに示すように、蛍光体セラミック板13の下面全体に反射膜23を形成する。この反射膜23は、蛍光体セラミック板13の下面に直接接して、すなわち、保護膜55を除去して蛍光体セラミック板13の下面に直接形成するようにしてもよいし、例えば、保護膜55がSiO膜のように透光性を有する場合には、蛍光体セラミック板13の下面に保護膜55を介して形成するようにしてもよい。なお、図6Dでは、保護膜55が透光性を有するものとして、反射膜23を蛍光体セラミック板13の下面に保護膜55を介して形成している。反射膜23としては、DBR(Distributed Bragg Reflector)膜等の誘電体多層膜、及び/又は、金属膜を用いることができる。反射膜23を構成する膜のうち最も上の膜がDBR膜の一部を構成する誘電体膜である場合、その最上の誘電体膜の屈折率と蛍光体セラミック板13中の蛍光体粒子17の屈折率との間の屈折率を有する膜を保護膜55として設けることが好ましい。なお、酸処理から蛍光体セラミック板13を保護するための保護膜55がSiO膜等、これらの屈折率の条件を満たさない材料の場合、一度保護膜55を除去した後、これらの条件を満たす保護膜55を形成しなおしてもよい。これにより、蛍光体粒子17が蛍光体セラミック板13の下面の一部を構成している場合に、その蛍光体粒子17からの光を保護膜55と最上の誘電体膜との界面で全反射することができる。これにより、蛍光体粒子17から直接的に入射する比較的高角度の光の量を低減させることができるため、そのような保護膜55を設けない場合と比較してDBR膜の積層数を減らすことができる。保護膜55及びDBR膜の最上の誘電体膜の厚さは、反射したい光の波長よりも大きくすることができ、例えば800nm以上とすることができる。保護膜55の厚さをDBR膜の最上の誘電体膜の厚さよりも大きくしてもよい。DBRを構成する誘電体膜の材料としては、Nb、Ta、ZrO又はSiO等が挙げられる。例えば、DBR膜の最上の誘電体膜がSiO膜であり蛍光体粒子17がYAG蛍光体である場合、それらの屈折率の間の屈折率を有する保護膜55の材料としては、Al、MgO又はGaが挙げられる。これらの保護膜55の材料は上記したDBR膜の材料よりも熱伝導率が高いため、これらのいずれかの材料で保護膜55を形成することにより、放熱性の向上という効果も期待できる。また、保護膜55と最上の誘電体膜との界面で全反射させる場合、保護膜55の厚みは、光学シミュレーションによって算出された最適な厚みよりも厚くしてもよい。これにより、それらの膜の界面で全反射が生じない確率を低減させることができると考えられる。
3. Reflective Film Forming Process After the acid treatment, as shown in FIG. 6D, a reflective film 23 is formed on the entire lower surface of the phosphor ceramic plate 13. The reflective film 23 may be directly in contact with the lower surface of the phosphor ceramic plate 13, i.e., the protective film 55 may be removed and formed directly on the lower surface of the phosphor ceramic plate 13, or, for example, when the protective film 55 is a SiO 2 film and has light-transmitting properties, the reflective film 23 may be formed on the lower surface of the phosphor ceramic plate 13 via the protective film 55. In FIG. 6D, the protective film 55 is assumed to have light-transmitting properties, and the reflective film 23 is formed on the lower surface of the phosphor ceramic plate 13 via the protective film 55. As the reflective film 23, a dielectric multilayer film such as a DBR (Distributed Bragg Reflector) film and/or a metal film can be used. When the uppermost film among the films constituting the reflective film 23 is a dielectric film constituting a part of the DBR film, it is preferable to provide a film having a refractive index between the refractive index of the uppermost dielectric film and the refractive index of the phosphor particles 17 in the phosphor ceramic plate 13 as the protective film 55. In addition, when the protective film 55 for protecting the phosphor ceramic plate 13 from the acid treatment is made of a material that does not satisfy these refractive index conditions, such as a SiO 2 film, the protective film 55 may be removed once and then re-formed to satisfy these conditions. As a result, when the phosphor particles 17 form a part of the lower surface of the phosphor ceramic plate 13, the light from the phosphor particles 17 can be totally reflected at the interface between the protective film 55 and the top dielectric film. As a result, the amount of light that is directly incident at a relatively high angle from the phosphor particles 17 can be reduced, so that the number of layers of the DBR film can be reduced compared to when such a protective film 55 is not provided. The thickness of the protective film 55 and the top dielectric film of the DBR film can be made larger than the wavelength of the light to be reflected, for example, 800 nm or more. The thickness of the protective film 55 may be made larger than the thickness of the top dielectric film of the DBR film. Examples of materials for the dielectric film that constitutes the DBR include Nb 2 O 5 , Ta 2 O 5 , ZrO 2 , and SiO 2 . For example, when the top dielectric film of the DBR film is a SiO2 film and the phosphor particles 17 are YAG phosphors, the material of the protective film 55 having a refractive index between those refractive indices can be Al2O3 , MgO , or Ga2O5 . Since these materials of the protective film 55 have a higher thermal conductivity than the above-mentioned materials of the DBR film, by forming the protective film 55 with any of these materials, it is expected that the effect of improving heat dissipation can be achieved. In addition, when total reflection is caused at the interface between the protective film 55 and the top dielectric film, the thickness of the protective film 55 may be made thicker than the optimal thickness calculated by optical simulation. It is considered that this can reduce the probability that total reflection does not occur at the interface between those films.

4.支持体接合工程
ここでは、蛍光体セラミック板13を下面側から支持する支持体33を、例えば、反射膜23上に接合する。支持体33は、例えば、窒化アルミニウムまたは銅からなる。この支持体33は蛍光体セラミック板13を支持または保護するものであって必要に応じて接合されるものであり、支持体接合工程は任意である。
4. Support Joining Step In this step, a support 33 that supports the phosphor ceramic plate 13 from the lower surface side is joined, for example, onto the reflective film 23. The support 33 is made of, for example, aluminum nitride or copper. This support 33 supports or protects the phosphor ceramic plate 13 and is joined as necessary, and the support joining step is optional.

以上のようにして作製された実施形態3の波長変換部材3に、透光性を有するマスク53を介して凸部13aの上面からそれぞれ蛍光体粒子17を励起する光を入射すると、入射光の少なくとも一部は、蛍光体を励起して、励起された蛍光体は、入射光とは異なる波長の光を発し、凸部13aの上面及びマスク53を介して外部に出射される。なお、マスク53は、凹部形成工程S2の後に除去されていてもよい。
以上のようにして、実施形態3の波長変換部材3は、マスク53を介して凸部13aの上面からそれぞれ入射した入射光の少なくとも一部を波長変換した後、凸部13aの上面及びマスク53を介して外部に出射させる。このとき、凸部13aの外周側面にはそれぞれ複数の凹部7が形成されているので、凸部13aの側面では光の出射が抑制されて凸部13aの内部に光を閉じ込めることができ、光出射面6とその外側との間の出射光の輝度差を大きくでき、かつ効率よく波長変換させることができる。
なお、実施形態3の波長変換部材3では、入射光の少なくとも一部を波長変換して出射させ、残りの一部を蛍光体セラミック13内で反射及び/又は散乱させて入射時と同じ波長のまま出射させるようにしてもよく、その場合には、入射光と同じ波長の光と波長変換後の入射光とは異なる波長の光との混色光が出射される。
When light that excites the phosphor particles 17 is incident on the upper surfaces of the convex portions 13a of the wavelength conversion member 3 of embodiment 3 produced as described above through the light-transmitting mask 53, at least a part of the incident light excites the phosphor, and the excited phosphor emits light of a wavelength different from that of the incident light, which is emitted to the outside through the upper surfaces of the convex portions 13a and the mask 53. The mask 53 may be removed after the recess formation step S2.
In this manner, the wavelength conversion member 3 of the third embodiment converts the wavelength of at least a portion of the incident light incident from the upper surface of the convex portion 13a through the mask 53, and then emits the light to the outside through the upper surface of the convex portion 13a and the mask 53. At this time, since a plurality of concave portions 7 are formed on each of the outer peripheral side surfaces of the convex portion 13a, the emission of light from the side surface of the convex portion 13a is suppressed, and the light can be confined inside the convex portion 13a, so that the luminance difference of the emitted light between the light emission surface 6 and the outside thereof can be increased, and the wavelength can be efficiently converted.
In addition, in the wavelength conversion member 3 of embodiment 3, at least a portion of the incident light may be wavelength converted and emitted, and the remaining portion may be reflected and/or scattered within the phosphor ceramic 13 to be emitted at the same wavelength as when it was incident. In this case, a mixture of light with the same wavelength as the incident light and light with a different wavelength from the incident light after wavelength conversion is emitted.

以上のようにして作製された実施形態3の波長変換部材3は、例えば、発光ダイオードや半導体レーザ素子等の励起光源と組み合わせることで、プロジェクター、照明、車両用灯具に用いることができる。また、例えば、支持体33に放熱機能を持たせることにより、光量の大きい光源の波長変換部材3として用いることができる。 The wavelength conversion member 3 of the third embodiment manufactured as described above can be used in projectors, lighting, and vehicle lamps by combining it with an excitation light source such as a light-emitting diode or a semiconductor laser element. In addition, for example, by providing the support 33 with a heat dissipation function, it can be used as the wavelength conversion member 3 for a light source with a large amount of light.

図6Fは、実施形態3の波長変換部材3を含む応用例の発光装置を模式的に示し、該発光装置は、波長変換部材3と波長変換部材3の凸部13aにレーザ光を照射するレーザダイオードである発光素子80とを含む。図6Fに示す発光装置において、発光素子80から出射されたレーザ光は、凸部13aの上面から入射され、入射光の少なくとも一部は蛍光体によって入射光とは異なる波長の光に変換されて凸部13aの上面から出射される。凸部13aの外周側面は、光の閉じ込めが向上した光反射面4となっているので、凸部13aの外周側面から漏れる光を少なくでき、凸部13aの上面から入射されたレーザ光を効率よく波長変換して、凸部13aの上面から出射させることができる。 Figure 6F shows a schematic diagram of a light-emitting device of an application example including the wavelength conversion member 3 of embodiment 3, and the light-emitting device includes the wavelength conversion member 3 and a light-emitting element 80 that is a laser diode that irradiates the convex portion 13a of the wavelength conversion member 3 with laser light. In the light-emitting device shown in Figure 6F, the laser light emitted from the light-emitting element 80 is incident on the upper surface of the convex portion 13a, and at least a part of the incident light is converted by the phosphor into light of a wavelength different from the incident light and emitted from the upper surface of the convex portion 13a. The outer peripheral side surface of the convex portion 13a is a light-reflecting surface 4 with improved light confinement, so that the amount of light leaking from the outer peripheral side surface of the convex portion 13a can be reduced, and the laser light incident on the upper surface of the convex portion 13a can be efficiently wavelength-converted and emitted from the upper surface of the convex portion 13a.

図6Fには、1つの発光素子80から1つの凸部13aにレーザ光を照射するように図示しているが、例えば、複数の発光素子80を備え、各発光素子80からそれぞれ対応する凸部13aに照射するように構成(構成1)してもよいし、1つの発光素子80により複数の凸部に13aに照射するように構成(構成2)してもよい。 In FIG. 6F, one light-emitting element 80 is shown irradiating laser light onto one convex portion 13a, but for example, multiple light-emitting elements 80 may be provided and each light-emitting element 80 may irradiate its corresponding convex portion 13a (configuration 1), or one light-emitting element 80 may be used to irradiate multiple convex portions 13a (configuration 2).

具体的には、構成1では、用途に応じて、発光素子80の数と凸部13aの数は異なっていてもよく、1つの発光素子80から2以上の凸部13aにレーザ光を照射するようにしてもよいし、2以上の発光素子80から1つの凸部13aにレーザ光を照射するようにしてもよい。
また、構成2では、用途に応じて、1つの発光素子80のレーザ光を、例えば、光学的に広げて一括して複数の凸部13aに照射するようにしてもよいし、例えば、方向制御が可能なミラー等を用いて、レーザ光を走査して時間的にずらして順次異なる凸部13aに照射するようにしてもよい。
Specifically, in configuration 1, the number of light-emitting elements 80 and the number of convex portions 13a may differ depending on the application, and laser light may be irradiated from one light-emitting element 80 to two or more convex portions 13a, or laser light may be irradiated from two or more light-emitting elements 80 to one convex portion 13a.
In addition, in configuration 2, depending on the application, the laser light of one light-emitting element 80 may be, for example, optically expanded and irradiated simultaneously onto a plurality of convex portions 13a, or the laser light may be scanned and shifted in time by using, for example, a mirror capable of controlling the direction, so that the laser light is irradiated sequentially onto different convex portions 13a.

実験例Experimental Example

実験例として、無機物粒子としてAl粒子を含み、蛍光体粒子としてYAG(Yttrium Aluminum Garnet)蛍光体粒子を含む焼結体を作製し、その焼結体の上面を酸処理した。そして、光を焼結体の下面から入射させたときの、焼結体の上面における光透過率を評価した。 As an experimental example, a sintered body containing Al 2 O 3 particles as inorganic particles and YAG (Yttrium Aluminum Garnet) phosphor particles as phosphor particles was prepared, and the upper surface of the sintered body was treated with acid. Then, the light transmittance of the upper surface of the sintered body was evaluated when light was incident from the lower surface of the sintered body.

具体的には、無機物粒子として、平均粒径が0.5μmの酸化アルミニウム粒子と、蛍光体粒子として、平均粒径が5μmのYAG蛍光体粒子を準備し、酸化アルミニウム粒子とYAG蛍光体粒子を8:2の割合で混合した。
混合は、湿式混合で24時間行った。
Specifically, aluminum oxide particles having an average particle size of 0.5 μm were prepared as inorganic particles, and YAG phosphor particles having an average particle size of 5 μm were prepared as phosphor particles, and the aluminum oxide particles and the YAG phosphor particles were mixed in a ratio of 8:2.
The mixing was carried out by wet mixing for 24 hours.

次に、混合粉体を柱形状に成形した。
成形は、ドクターブレード法を用いてグリーンシートを一次成形した後、一次成形品をカッターを用いて柱形状に二次成形した。
The mixed powder was then formed into a cylinder shape.
The green sheet was primarily molded using a doctor blade method, and the primarily molded product was then secondarily molded into a columnar shape using a cutter.

次に、成形品を焼結した。
焼結は、1400℃の温度で5時間大気中で常圧焼結法により一次焼結させた後、1400℃の温度で10時間不活性ガス雰囲気でアニール(熱処理)した。
The moulded part was then sintered.
The sintering was carried out by primary sintering in the atmosphere at a temperature of 1400° C. for 5 hours by atmospheric sintering, and then annealing (heat treatment) was carried out in an inert gas atmosphere at a temperature of 1400° C. for 10 hours.

焼結後、焼結体を酸処理し、焼結体の上面に複数の凹部を形成した。
酸処理は、燐酸と硫酸が1:3の割合で混合された混合液を180℃に加熱して焼結体を入れ、その後、さらに別の同じ混合液の温度を300℃にしたものへ焼結体を入れ、10分間経過した後、180℃の混合液へ焼結体を入れ、徐々に温度を下げて取り出した。
After sintering, the sintered body was subjected to an acid treatment to form a plurality of recesses on the upper surface of the sintered body.
For the acid treatment, a mixed liquid of phosphoric acid and sulfuric acid in a ratio of 1:3 was heated to 180°C and the sintered body was placed in it. Thereafter, the sintered body was placed in another mixed liquid of the same type but at a temperature of 300°C. After 10 minutes had elapsed, the sintered body was placed in the mixed liquid at 180°C, and the temperature was gradually lowered before being removed.

酸処理した焼結体を水洗した後、光を焼結体の下面から入射させ、焼結体の上面における光透過率を測定した。
光透過率は、分光光度計により測定した。
After the acid-treated sintered body was washed with water, light was made to enter the bottom surface of the sintered body, and the light transmittance at the top surface of the sintered body was measured.
The light transmittance was measured by a spectrophotometer.

また、アニールまで実施例と同様にして作製し、酸処理を行っていない比較例の焼結体を実験例と同様にして光透過率を測定した。 In addition, the sintered body of the comparative example was prepared in the same manner as the example up to the annealing step, and the light transmittance was measured in the same manner as the experimental example, without undergoing acid treatment.

その結果、実験例の焼結体の上面の光透過率は、540nmで55%であるのに対して、比較例の焼結体の上面の光透過率は、540nmで60%であった。つまり、実験例の焼結体の上面の光透過率が、比較例の実験例の焼結体の上面の光透過率よりも低くなっており、実験例の焼結体の上面において、比較例と比べて光の閉じ込めが向上していることがわかった。 As a result, the light transmittance of the top surface of the sintered body of the experimental example was 55% at 540 nm, whereas the light transmittance of the top surface of the sintered body of the comparative example was 60% at 540 nm. In other words, the light transmittance of the top surface of the sintered body of the experimental example was lower than the light transmittance of the top surface of the sintered body of the comparative example, and it was found that the light confinement was improved in the top surface of the sintered body of the experimental example compared to the comparative example.

また、実験例と同様にして作製した焼結体11aの光反射面4に反射部材21aを形成したときの断面写真を図7Aに示す。図7Aに示すように、光反射面4における蛍光体粒子17の分布が、焼結体11aの内部における蛍光体粒子17の分布より少ないことが確認された。また、焼結体11aの凹部7に反射部材21aが侵入し、反射部材21aの凸部8が形成されることが確認された。また、図7Bには、光反射面4の形状が理解しやすいように、図7Aから反射部材21aを除いた断面写真を示す。図7Bに示すように、焼結体11aの凹部7と反射部材21aの凸部8の間に空隙9が残っていることが確認された。ここで、反射部材21aは、スリップキャスト法を用い、焼結体11a周辺に反射部材21aとなるスラリーを流し込み、乾燥させたのち、大気雰囲気で1400℃、1時間熱処理をして形成した。 Figure 7A shows a cross-sectional photograph of the reflective member 21a formed on the light-reflecting surface 4 of the sintered body 11a produced in the same manner as in the experimental example. As shown in Figure 7A, it was confirmed that the distribution of phosphor particles 17 on the light-reflecting surface 4 was less than the distribution of phosphor particles 17 inside the sintered body 11a. It was also confirmed that the reflective member 21a penetrated into the recessed portion 7 of the sintered body 11a, and the protruding portion 8 of the reflective member 21a was formed. Figure 7B shows a cross-sectional photograph of the reflective member 21a removed from Figure 7A so that the shape of the light-reflecting surface 4 can be easily understood. As shown in Figure 7B, it was confirmed that a gap 9 remains between the recessed portion 7 of the sintered body 11a and the protruding portion 8 of the reflective member 21a. Here, the reflective member 21a was formed by using a slip casting method, pouring a slurry to become the reflective member 21a around the sintered body 11a, drying it, and then heat-treating it at 1400 ° C. in an air atmosphere for 1 hour.

これに対して、酸処理を行っていない比較例の焼結体の光反射面に反射部材を形成した場合には、図7Cに示すように、光反射面における蛍光体粒子の分布と、焼結体の内部における蛍光体粒子の分布との間に差はみられなかった。また、実験例で確認されたような反射部材が侵入した凹部は確認されなかった。 In contrast, when a reflective member was formed on the light-reflecting surface of the sintered body of the comparative example that had not been subjected to acid treatment, as shown in Figure 7C, no difference was observed between the distribution of phosphor particles on the light-reflecting surface and the distribution of phosphor particles inside the sintered body. Furthermore, no recesses where the reflective member had entered were observed, as was the case in the experimental example.

1、2、3 波長変換部材
4 光反射面
5 光入射面
6 光出射面
7 凹部
8 凸部
9 空隙
11、11a 焼結体
12 焼結体(蛍光体セラミック板)
12a 焼結体(凸部)
12b ベース部
13 焼結体(蛍光体セラミック板)
13a 凸部
17 蛍光体粒子
18 ガラス
21、21a、22 反射部材
23 反射膜
33 支持体
53 マスク
55 保護膜
80 発光素子
L4 線
L40 仮想線
REFERENCE SIGNS LIST 1, 2, 3 Wavelength conversion member 4 Light reflecting surface 5 Light incident surface 6 Light emitting surface 7 Concave portion 8 Convex portion 9 Void 11, 11a Sintered body 12 Sintered body (phosphor ceramic plate)
12a Sintered body (protruding portion)
12b Base portion 13 Sintered body (phosphor ceramic plate)
13a: convex portion 17: phosphor particle 18: glass 21, 21a, 22: reflective member 23: reflective film 33: support 53: mask 55: protective film 80: light emitting element L4: line L40: imaginary line

Claims (10)

光入射面と、光出射面と、前記光入射面及び光出射面とは異なる面である光反射面とを備える焼結体を含む波長変換部材の製造方法であって、
無機物粒子と蛍光体粒子とを含む焼結体を準備する焼結体準備工程と、
前記焼結体を酸処理し、前記焼結体の光反射面に複数の凹部を形成する凹部形成工程と、
前記焼結体の外周側面が前記光反射面であって、該外周側面に接しかつ前記光入射面及び光出射面を露出させるように反射部材を設ける反射部材配置工程と、を含み、
前記反射部材配置工程は、
反射部材用粉体を、前記複数の凹部を形成した焼結体を取り囲むように一体的に成形することと、
前記反射部材用粉体及び複数の凹部を形成した焼結体を一体的に焼結することと、
を含むことを特徴とする波長変換部材の製造方法。
A method for producing a wavelength conversion member including a sintered body having a light incident surface, a light exit surface, and a light reflecting surface that is different from the light incident surface and the light exit surface, comprising:
a sintered body preparation step of preparing a sintered body containing inorganic particles and phosphor particles;
a recess forming step of treating the sintered body with acid to form a plurality of recesses on a light reflecting surface of the sintered body;
a reflecting member disposing step of disposing a reflecting member on the outer peripheral side surface of the sintered body, the outer peripheral side surface being the light reflecting surface, the reflecting member being in contact with the outer peripheral side surface and exposing the light incident surface and the light exit surface;
The reflective member arrangement step includes:
forming a powder for a reflecting member integrally with the sintered body having the plurality of recesses formed therein;
sintering the powder for reflection member and the sintered body having the plurality of recesses integrally;
A method for producing a wavelength conversion member, comprising :
前記凹部形成工程において、前記焼結体の光入射面及び/又は光出射面に複数の凹部を形成し、
前記凹部形成工程後に、
前記光入射面及び/又は光出射面の凹部を除去する凹部除去工程を含む請求項1に記載の波長変換部材の製造方法。
In the recess forming step, a plurality of recesses are formed on a light incident surface and/or a light emitting surface of the sintered body,
After the recess forming step,
The method for producing a wavelength conversion member according to claim 1 , further comprising a recess removing step of removing recesses on the light incident surface and/or the light exit surface.
前記焼結体は柱形状である
請求項1または2に記載の波長変換部材の製造方法。
The sintered body has a columnar shape .
A method for producing the wavelength conversion member according to claim 1 or 2.
前記焼結体準備工程において、前記焼結体を2以上準備し、
前記反射部材配置工程は、
前記反射部材用粉体を、前記複数の凹部を形成した焼結体をそれぞれ取り囲むように一体的に成形することと、
前記反射部材用粉体及び複数の凹部を形成した焼結体を一体的に焼結することで波長変換部材集合体を作製すること
を含み、
前記波長変換部材集合体を、それぞれの前記波長変換部材が前記1又は2以上の焼結体を含むように複数に分割する個片化工程を含む請求項1~3のいずれか1項に記載の波長変換部材の製造方法。
In the sintered body preparation step, two or more sintered bodies are prepared,
The reflective member arrangement step includes:
forming the powder for the reflecting member integrally so as to surround each of the sintered bodies having the plurality of recesses;
The powder for the reflection member and the sintered body having the plurality of recesses formed therein are integrally sintered to produce a wavelength conversion member assembly,
The method for producing a wavelength conversion member according to any one of claims 1 to 3, further comprising a singulation step of dividing the wavelength conversion member assembly into a plurality of wavelength conversion members each including the one or more sintered bodies.
前記凹部形成工程において、前記焼結体の光入射面及び/又は光出射面にマスクを形成し、該マスクから露出された表面に複数の凹部を形成する請求項1に記載の波長変換部材の製造方法。 The method for manufacturing a wavelength conversion member according to claim 1, wherein in the recess forming step, a mask is formed on the light incident surface and/or the light exit surface of the sintered body, and multiple recesses are formed on the surface exposed from the mask. 前記光入射面及び光出射面は同一の表面からなる請求項1~のいずれか1項に記載の波長変換部材の製造方法。 The method for producing a wavelength conversion member according to any one of claims 1 to 5 , wherein the light incident surface and the light exit surface are formed by the same surface. 光入射面と、光出射面と、前記光入射面及び光出射面とは異なる面である光反射面とを有し、蛍光体粒子を含む焼結体と、前記焼結体の外周側面が前記光反射面であって、該外周側面に接しかつ前記光入射面及び光出射面を露出させるように設けられた反射部材と、を備え、前記焼結体と前記反射部材とが一体的に焼結されている波長変換部材であって、
前記焼結体の光反射面は、複数の凹部を有し、
前記光反射面における蛍光体粒子の分布は、前記焼結体の内部における蛍光体粒子の分布より少ないことを特徴とする波長変換部材。
a sintered body having a light incident surface, a light exit surface, and a light reflecting surface which is different from the light incident surface and the light exit surface, the sintered body including phosphor particles; and a reflecting member provided in contact with the outer peripheral side surface so as to expose the light incident surface and the light exit surface, the sintered body and the reflecting member being sintered integrally ,
The light reflecting surface of the sintered body has a plurality of recesses,
A wavelength conversion member, characterized in that the distribution of phosphor particles on the light reflecting surface is smaller than the distribution of phosphor particles inside the sintered body.
前記焼結体の周縁領域において、前記焼結体に囲まれた空隙を有することを特徴とする請求項に記載の波長変換部材。 The wavelength conversion member according to claim 7 , further comprising a void surrounded by the sintered body in a peripheral region of the sintered body. 記反射部材の内周側面の一部が該外周側面に接している請求項7または8に記載の波長変換部材。 The wavelength conversion member according to claim 7 or 8 , wherein a part of an inner peripheral side surface of the reflecting member is in contact with the outer peripheral side surface. 2以上の前記焼結体の光入射面及び/又は光出射面が略同一面上に位置するように一体で形成されたことを特徴とする請求項7~9のいずれか1項に記載の波長変換部材。 The wavelength conversion member according to any one of claims 7 to 9, characterized in that the light entrance surface and/or the light exit surface of two or more of the sintered bodies are integrally formed so as to be positioned on approximately the same plane.
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